- Advanced Idea Mechanics (A.I.M.): A terrorist organization of scientists dedicated to world power and the overthrow of all government through a technological revolution.
- Americop: A former police officer turned ruthless vigilante.
- Ameridroid: A 20-foot tall android, built to resemble Captain America, controlled by the brain of former Nazi spy Lyle Dekker.
- Armadillo: A super-powered criminal with an armadillo's physiology.
- Arnim Zola: Nazi biochemist who became the first human genetic engineer in history.
- Baron Blood: John Falsworth, a British aristocrat, who sought out Count Dracula.
- Baron von Strucker: The founder of HYDRA and longtime foe of both Captain America and Nick Fury's S.H.I.E.L.D.
- Baron Zemo: Heinrich Zemo was one of the elite Nazi scientists during World War II. After his death, his son Helmut Zemo took on the role and continued a heated rivalry with Captain America; he has teetered between heroics and villainy due to his association with the Thunderbolts, an ultimately-reformed version of the Masters of Evil that took on false hero guises in the 1990s absence of the Fantastic Four, Avengers and other high-profile heroes.
- Batroc the Leaper: A French mercenary and leader of his own brigade of criminals, Batroc's Brigade.
- Black Talon I: A World War II era criminal mastermind and Nazi sympathizer.
- Blackwing: Costumed super-villain and the son of Silvermane, also a former member of the Skeleton Crew.
- Blistik: A tech-based vigilante who stood for "the quality of life" of the residents of New York City.
- Blue Streak: Former spy turn costumed operative of the subversive organization called The Corporation.
- Cache: A super computer come to life with ultimate knowledge of any data that is in the internet universe.
- Cold War: An ice manipulator created by Al Milgrom
- The Corporation: A business-like criminal organization, which employed numerous super-villains against heroes across the nation. Captain America did battle with many of their surrogates, including Blue Streak, Night Flyer, Ameridroid and Vamp/Animus.
- Crime Wave: A short lived union of costumed super-villains (The Eel, Plantman, Scarecrow, Porcupine and the Viper) under the leadership of the Cowled Commander.
- Crossbones: The chief henchman of the Red Skull. Publicly responsible for the assassination of Steve Rogers in the aftermath of the superhero Civil War.
- Cutthroat: Costumed super-villain once associated with the Red Skull's Skeleton Crew. He is the brother of former Serpent Society member (and Captain America paramour) Diamondback.
- Dead Ringer: A criminal who uses his power of necromimickry to take on the appearance and abilities of deceased individuals. Friend and former ally of Mike Farrell, the second Super-Patriot 
- Death-Throws: A team of five costumed jugglers (Bombshell, Knickknack, Oddball, Ringleader & Tenpin) who used their skills to commit crime.
- Doctor Faustus: A psychiatrist and criminal mastermind, commonly allied with the Red Skull and Arnim Zola. His psychological manipulation of Sharon Carter led to her killing Steve Rogers.
- Dredmund the Druid: A master in the magical and mystical arts bent on world domination. Attained the power of the Moongem and for a short time became the Starwolf.
- Dr. Cedric Rawlings: A former mad scientist who developed rocket technology for the Nazis.
- Dr. Octopus: A sometimes enemy of Cap, also Daredevil Fantastic 4, and most frequently, Spider-Man.
- Everyman: A self-professed "defender of the common people". Later went by the name Zeitgeist.
- Flag-Smasher: A Swiss terrorist, determined to unite the world by destroying nationalities.
- Hate-Monger: A clone of Adolf Hitler.
- Heinz Kruger: The Nazi agent who murdered Dr. Erskine after the process that turned Steve Rogers into Captain America was completed.
- HYDRA: A criminal organization dedicated to the achievement of world domination through terrorist and subversive activities on various fronts, resulting in a fascist New World Order.
- Jack O'Lantern: Former member of the Skeleton Crew. One of several individuals (mainly connected to Spider-Man) who used the Jack O'Lantern moniker.
- Karl Stryker: A Nazi sympathizer who used a hydraulics-powered combat suit to combat Captain America. His son Viktor took revenge on Captain American soon after, but was killed in the process.
- King Cobra: Costumed super-villain, known for a phenomenal (mutated) mastery of his musculature in combat situations, and member of the original Serpent Squad. Also worked commonly alongside Mister Hyde against Captain America and other heroes.
- Kligger: Former leader of The Corporation, the criminal guise of Senator Eugene Stivak. Often accompanied by his aide Veda (who he personally killed when she eventually gave up her allegiance to the organization)
- Machinesmith: A master robot-maker (once a villain known as Starr Saxon) who became a living, cybernetic-system program (artificial consciousness), equipped to transmit itself into virtually any electronics system at will.
- Madame Hydra: Leader of HYDRA. She is also known as the second Viper.
- Master Man: A Nazi super-soldier who, like Steve Rogers, was enhanced by a Nazi-version of the American super-soldier serum.
- Minister Blood: Hypnotist agent of the Red Skull. Brother of Mother Night.
- Mister Hyde: Chemically enhanced super-villain. Worked commonly alongside King Cobra against superheroes, especially Captain America.
- MODAM (Mental Organism Designed for Aggressive Maneuvers): An A.I.M. agent who, like MODOK, was originally a tech agent for the organization mutated for various offensive measures against their enemies.
- MODOK (Mental Organism Designed Only for Killing): A former A.I.M. tech transformed with advanced mutagenics into the organization's leader. Later disassociated itself from A.I.M. and works alongside other "genius-level" villains in the Marvel Universe.
- Mother Night: Ally of the Red Skull and Crossbones, former leader of the Sisters of Sin and former member of the Skeleton Crew. Sister of Minister Blood.
- Nefarius: Affiliated with the Secret Empire, he planned to damage Cap's reputation by accusing him of vigilantism.
- Porcupine: A weapons designer clad in "porcupine-like" battle armor.
- Red Skull: Captain America's archenemy, a Nazi super-soldier and Hitler's successor.
- Red Guardian: Soviet equivalent to Captain America and a Cold War rival.
- Scourge of the Underworld: A cadre of super-villain killers originally tackled and often confronted by Captain America and his allies.
- Secret Empire: A terrorist organization, led by a series of individuals called Number One (one of whom was implied to be a very high level U.S. government official).
- Sensational Hydra: A Skrull infiltrator of HYDRA, who battled Captain America and the Avengers.
- Serpent Squad: A group of snake-themed super-villains.
- Serpent Society: A larger group of snake-themed super-villains.
- Sidewinder: The creator and original leader of the Serpent Society. The original Sidewinder, Seth Voelker, has since retired and reformed; he has been succeeded in the costume by at least 2 others.
- Sisters of Sin: A quasi-religious cult, created by the Red Skull, that promoted hatred and violence.
- Sin: Daughter of the Red Skull.
- Sleeper: A series of robots designed and entombed by Nazi Germany to wreak havoc on society in future years.
- Superia: Leader of The Femizons, a group of female super-villains. Later a member of Norman Osborn's Dark Avengers.
- Super Patriot: John Walker was Captain America's replacement during the 1980s (when his removal from the heroic role was orchestrated by The Red Skull). He was an unwitting rival to Steve Rogers but nonetheless a hero in his own right, and ultimately he became an ally to Captain America as the renamed U.S. Agent.
- Swine: Hector Santiago, the dictator of Rio De Muerte ("River of Death"), slavemaster and leader of a small private army.
- Taskmaster: Costumed super villain with the uncanny ability to replicate his enemies' fighting techniques. Also a trainer of super-villains, employed by criminal organizations and other villains.
- The Man With No Face: Created by Zhang Chin and failed as an experiment in 1950. Villain to the new Captain America.
- Tumbler: A costumed criminal acrobat.
- Ultimatum: A terrorist organization headed by Flag-Smasher.
- Vamp: A former member of The Corporation, who briefly infiltrated SHIELD as a super-powered hero. She possessed a monstrous alter-ego called Animus.
- Vermin: Former geneticist mutated by Baron Zemo and Primus into a murderous rat-like creature.
- Viper: Costumed villain, brother of the Eel.
- The Watchdogs: A racially-motivated terrorist organization opposed to controversial subjects in American culture.
- Walking Stiletto: A robot supervillain created by A.I.M.
- Winter Soldier: Codename used for Cap's former WWII partner Bucky Barnes, who, though thought dead, was a notorious, mysterious Soviet assassin for decades. Ultimately overcame his Soviet reprogramming to become Cap's ally (and for a time the new Captain America) once again.
- Yellow Claw: Criminal mastermind of Communist China.
- Captain America Comics #9, Young Allies #2
- Captain America Vol.1 #422
- Captain America Vol. 3 #34-39
- Marvel Comics Presents #2
- Captain America Vol.1 #157-159
- Captain America #425-427, 439
- Tales of Suspense #69-71
- Marvel Fanfare Vol.1 #5
- Captain America Vol.3 #5-7
- Captain America Vol.1 #206-208
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