| • Fred Tatasciore | voiced | Dr. Franklin Hall a.k.a Graviton / Frost Giant #2 / Mandrill / Yon Rogg / SHIELD Agent / AIM Pilot / Comm Officer / Volstagg / Fenric / Ben Grimm a.k.a The Thing / Red Hulk | 16 Episodes |
| • Jennifer Hale | voiced | Carol Danvers / Carol Danvers a.k.a Ms. Marvel / Carol Danvers a.k.a Ms. Marvel | Corrina | 14 Episodes |
| • Kari Wahlgren | voiced | Jane Foster / Enchantress / Karnilla | 14 Episodes |
| • Troy Baker | voiced | Clay Quartermain / Clay Quartermain | Blizzard | Whirlwind / Blizzard / Whirlwind / Grey Gargoyle / Donald Gill a.k.a. “Blizzard” / Farade / Lilk / Sydren / Michael Korvac | Groot / Clay Quartermain | Skrull Interrogator / Clay Quartermain | Major Talbot | SHIELD Agent / Clay Quartermain | Robbie Robertson | 14 Episodes |
| • Rick D. Wasserman | voiced | Damocles / Carl Creed a.k.a. Absorbing Man / Frost Giant #1 / Surtur / Skrull Commander | 12 Episodes |
| • Wally Wingert | voiced | Ultron / MODOC / Yellowjacket | 10 Episodes |
| • Vanessa Marshall | voiced | Natasha Romanoff a.k.a Black Widow | Madame Viper / Natasha Romanoff a.k.a Black Widow | SHIELD Computer | Waitress / Natasha Romanoff a.k.a Black Widow | Madame Viper | Hydra Computer / Natasha Romanoff a.k.a Black Widow | AIM Computer / Natasha Romanoff a.k.a Black Widow / Madame Viper / Madame Viper | Anaconda | 10 Episodes |
| • Robin Atkin Downes | voiced | Abomination / Baron Zemo / Abomination | Baron Zemo | 9 Episodes |
| • Kari Wuhrer | voiced | Maria Hill | 9 Episodes |
| • Gabriel Mann | voiced | Bruce Banner | 8 Episodes |
| • Chris Cox | voiced | Crimson Dynamo / HYDRA Soldier #2 / Fandral / Agent McCarthy / Rattler / Peter Corbeau | 8 Episodes |
| • Phil LaMarr | voiced | SHIELD Doctor / Cameraman / Simon Williams a.k.a Wonder Man / Child Kang | 7 Episodes |
| • Jim Ward | voiced | Baron Von Strucker / SHIELD Agent / Damocles / 1940's Announcer / AIM Scientist / HYDRA Soldier #1 / Henry Gyrich | Damocles / Henry Gyrich | Skrull | 7 Episodes |
| • Nolan North | voiced | Balder / Scientist Supreme / Jimmy Woo / Living Laser / Pile Driver / Dispatch / Chemistro / A.I.M. Scientist Supreme / Chemistro | Balder | 7 Episodes |
| • James Mathis III | voiced | Bulldozer / King Cobra / Dark Captain / Kree Black Ops Commander | 7 Episodes |
| • Cam Clarke | voiced | Doctor Leonard Samson / Vector / Constrictor | 6 Episodes |
| • Steven Jay Blum | voiced | Red Skull / Logan / Hydra Scientist / Ogre / Beta Ray Bill / Dell Rusk / Wolverine | 6 Episodes |
| • Jonathan Adams | voiced | Kang the Conqueror | 5 Episodes |
| • Jeffrey Combs | voiced | Leader | 5 Episodes |
| • Elizabeth Daily | voiced | Bobbi Morse a.k.a Mockingbird / Queen Veranke | 5 Episodes |
| • Tom Kane (1) | voiced | Ultron / Jasper Sitwell / Professor Thornton | 5 Episodes |
| • Peter Jessop (1) | voiced | Vision | 5 Episodes |
| • Roger Craig Smith | voiced | Phillip Lawson a.k.a. Captain Marvel | 5 Episodes |
| • Nika Futterman | voiced | Sif / Hela | 4 Episodes |
| • Lance Henriksen | voiced | Grim Reaper | 4 Episodes |
| • Graham McTavish | voiced | Loki | 4 Episodes |
| • Dawn Olivieri | voiced | Pepper Potts | 4 Episodes |
| • Erin Torpey | voiced | Sue Storm a.k.a The Invisible Woman | 4 Episodes |
| • J. B. Blanc | voiced | Wrecker / Heimdall / Frost Giant #1 / Wrecker | Police Officer | 4 Episodes |
| • Jon Curry (1) | voiced | Winter Soldier / Winter Soldier | Colonel Tom Parker | 3 Episodes |
| • Clancy Brown | voiced | Odin / Troll | 3 Episodes |
| • David Kaufman | voiced | Johnny Storm a.k.a The Human Torch | 3 Episodes |
| • Bumper Robinson | voiced | James “Rhodey” Rhodes | 3 Episodes |
| • Colleen O'Shaughnessey | voiced | Vapor / Cassie Lang / Jocasta | 3 Episodes |
| • Drake Bell | voiced | Peter Parker a.k.a Spider-Man | 3 Episodes |
| • Keith Ferguson | voiced | General Thaddeus “Thunderbolt” Ross | 3 Episodes |
| • Christopher B. Duncan | voiced | Luke Cage | 2 Episodes |
| • Mark Hamill | voiced | Ulysses Klaw | 2 Episodes |
| • Alex Desert | voiced | Damocles Officer / Jack Fury | 2 Episodes |
| • Kevin Michael Richardson | voiced | Man Ape / N'Gassi | 2 Episodes |
| • Lex Lang | voiced | Victor von Doom a.k.a Doctor Doom | 2 Episodes |
| • Scott Menville | voiced | Bucky | 2 Episodes |
| • Dee Bradley Baker | voiced | Reed Richards a.k.a Mr. Fantastic | 2 Episodes |
| • Danny Mann | voiced | Mad Thinker | 2 Episodes |
| • Loren Lester | voiced | Danny Rand a.k.a Iron Fist | Newscaster / Danny Rand a.k.a Iron Fist | 2 Episodes |
| • Gary Anthony Williams | voiced | Thunderball | 2 Episodes |
| • Kyle Hebert | voiced | Loki / Kl'rt a.k.a Super-Skrull | 2 Episodes |
| • Mary Elizabeth McGlynn | voiced | Abigail Brand | 2 Episodes |
| • Lance Reddick | voiced | Falcon | 2 Episodes |
| • Grant Moninger | voiced | Armin Zola / Doughboy | 2 Episodes |