| Chris Evans | .... | Captain America / Steve Rogers |
| Hayley Atwell | .... | Peggy Carter |
| Sebastian Stan | .... | James Buchanan 'Bucky' Barnes |
| Tommy Lee Jones | .... | Colonel Chester Phillips |
| Hugo Weaving | .... | Johann Schmidt / Red Skull |
| Dominic Cooper | .... | Howard Stark |
| Richard Armitage | .... | Heinz Kruger |
| Stanley Tucci | .... | Dr. Abraham Erskine |
| Samuel L. Jackson | .... | Nick Fury |
| Toby Jones | .... | Dr. Arnim Zola |
| Neal McDonough | .... | Timothy 'Dum Dum' Dugan |
| Derek Luke | .... | Gabe Jones |
| Kenneth Choi | .... | Jim Morita |
| JJ Feild | .... | James Montgomery Falsworth |
| Bruno Ricci | .... | Jacques Dernier |
| Lex Shrapnel | .... | Gilmore Hodge |
| Michael Brandon | .... | Senator Brandt |
| Martin T. Sherman | .... | Brandt's Aide |
| Natalie Dormer | .... | Pvt. Lorraine |
| Oscar Pearce | .... | Search Team Leader |
| William Hope | .... | S.H.I.E.L.D. Lieutenant |
| Nicholas Pinnock | .... | S.H.I.E.L.D. Tech |
| Marek Oravec | .... | Jan |
| David Bradley | .... | Tower Keeper |
| Leander Deeny | .... | Barman |
| Sam Hoare | .... | Nervous Recruit |
| Simon Kunz | .... | 4F Doctor |
| Kieran O'Connor | .... | Loud Jerk |
| Jenna-Louise Coleman | .... | Connie |
| Sophie Colquhoun | .... | Bonnie |
| Doug Cockle | .... | Young Doctor |
| Ben Batt | .... | Enlistment Office MP |
| Mollie Fitzgerald | .... | Stark Girl |
| Damon J. Driver | .... | Sergeant Duffy |
| David McKail | .... | Johann Schmidt's Artist |
| Amanda Walker | .... | Antique Store Owner |
| Richard Freeman | .... | SSR Doctor |
| Katherine Press | .... | Project Rebirth Nurse |
| Sergio Covino | .... | Kruger's Aide |
| Marcello Walton | .... | Undercover Bum |
| Vincent Montuel | .... | Undercover Bum |
| Fabrizio Santino | .... | Kruger's Driver |
| Maxwell Newman | .... | Boy at Dock |
| Anatole Taubman | .... | Roeder |
| Jan Pohl | .... | Hutter |
| Erich Redman | .... | Schneider |
| Rosanna Hoult | .... | The Star Spangled Singer |
| Naomi Slights | .... | The Star Spangled Singer |
| Kirsty Mather | .... | The Star Spangled Singer |
| Megan Sanderson | .... | Kid in USO Audience |
| Darren Simpson | .... | Kid in USO Audience |
| Fernanda Toker | .... | Newsstand Mom |
| Laura Haddock | .... | Autograph Seeker |
| James Payton | .... | 'Adolph Hitler' |
| Ronan Raftery | .... | Army Heckler |
| Nick Hendrix | .... | Army Heckler |
| Luke Allen-Gale | .... | Army Heckler |
| Jack Gordon | .... | Army Heckler |
| Ben Uttley | .... | HYDRA Guard / HYDRA Pilot |
| Kevin Millington | .... | Stark's Engineer |
| Patrick Monckeberg | .... | Manager Velt |
| Peter Stark | .... | HYDRA Lieutenant |
| Amanda Righetti | .... | S.H.I.E.L.D. Agent |
| Jennifer Abbotts | .... | USO Dancer |
| Michelle Antrobus | .... | USO Dancer |
| Lucy Dean | .... | USO Dancer |
| Erin Dusek | .... | USO Dancer |
| Nicole Evans | .... | USO Dancer |
| Lizzi Franklin | .... | USO Dancer |
| Emma Harris | .... | USO Dancer |
| Rachael Isherwood | .... | USO Dancer |
| Danielle Kelly | .... | USO Dancer |
| Nicole May | .... | USO Dancer |
| Stevie-Jean McGuire | .... | USO Dancer |
| Anna McNicholas | .... | USO Dancer |
| Rosie Pethullis | .... | USO Dancer |
| Jessica Powell | .... | USO Dancer |
| Rachel Quartley | .... | USO Dancer |
| Sarah Riches | .... | USO Dancer |
| Holly Rostron | .... | USO Dancer |
| Caroline Royce | .... | USO Dancer |
| Stephanie Jayne Thompson | .... | USO Dancer |
| Lucie Waugh | .... | USO Dancer |
| Billy Lozowski | .... | USO Drummer |
| Gregory Paulett | .... | USO Drummer |
| Adam Birch | .... | USO Drummer |
| Adam Kent | .... | USO Drummer |
| William Morris | .... | USO Drummer |
| David Sdall | .... | USO Drummer |
| Paul Simmons | .... | USO Drummer |
| Marc Wheeler | .... | USO Drummer |
| Chris Diggle | .... | USO Drummer |
| Michael Humphrey | .... | USO Drummer |
| Raed Abbas | .... | Prisoner of War (uncredited) |
| Esme Allen-Quarmby | .... | New York Child (uncredited) |
| Colin Alltree | .... | Senator Security (uncredited) |
| Michael Aston | .... | Businessman (uncredited) |
| Paul Bergquist | .... | Bookshop Owner (uncredited) |
| Christian Black | .... | Sgt. Buck (uncredited) |
| Paul Blackwell | .... | Soldier (uncredited) |
| Mark Callum | .... | Newspaper Stole Holder (uncredited) |
| Will Carlson | .... | Reporter (uncredited) |
| James Chahine | .... | Army Heckler (uncredited) |
| Will Chambers | .... | Docker (uncredited) |
| David Chant | .... | U.S. Solider (uncredited) |
| Jason Alexander Charchan | .... | German Soldier (uncredited) |
| Robert Clayton | .... | US Marine 4th Battalion (uncredited) |
| Jack Conway | .... | S.H.I.E.L.D. Agent (uncredited) |
| James Cook | .... | 1st Flight Lieutenant - Stark Expedition (uncredited) |
| James Currie | .... | Commando (uncredited) |
| Graham Curry | .... | US Marine 4th Battalion (uncredited) |
| Eddie Davenport | .... | HYDRA Soldier (uncredited) |
| Paul Davies | .... | Hydra Soldier (uncredited) |
| Liam Elcoat | .... | Brooklyn Pedestrian (uncredited) |
| Joshua Ferdinand | .... | US Marine (uncredited) |
| Scott Ford | .... | German Soldier (uncredited) |
| Salo Gardner | .... | (uncredited) |
| Spencer Garrett | .... | Newsreel Announcer (uncredited) |
| Joe Garvey | .... | HYDRA Guard (uncredited) |
| Rich Goble | .... | Italian Soldier (uncredited) |
| Drew Gregory | .... | SHIELD Agent (uncredited) |
| Salem Hanna | .... | Russian POW (uncredited) |
| James Hare | .... | US Marine (uncredited) |
| Michael Hennessy | .... | Customer / Pub Singer (uncredited) |
| Leigh Holland | .... | US Soldier (uncredited) |
| Jacqueline Honulik | .... | Model in Modern NYC (uncredited) |
| Vera Horton | .... | 1930th Citizen (uncredited) |
| Tim Howard | .... | Soldier (uncredited) |
| Sonja Isabella | .... | Officer's Wife (uncredited) |
| Tobias James-Samuels | .... | Producer / Soldier (uncredited) |
| Todd Von Joel | .... | Hydra Soldier (uncredited) |
| Jacob Johnston | .... | HYDRA Soldier (uncredited) |
| Chris Jorie | .... | Reporter (uncredited) |
| John Samuel Kande | .... | US Soldier (uncredited) |
| Matt Kohler | .... | HYDRA Soldier (uncredited) |
| Stan Lee | .... | General (uncredited) |
| Steve Leighton | .... | Brooklyn Tour Guide (uncredited) |
| Addison LeMay | .... | SHIELD Agent X (uncredited) |
| Alan Mandel | .... | Prisoner of War (uncredited) |
| Josh Margulies | .... | Brooklyn Pedestrian (uncredited) |
| Anthony Milton | .... | US Soldier (uncredited) |
| Michael Mulqueen | .... | Hydra Infantry (uncredited) |
| Brian Niblett | .... | Theatre Spectator (uncredited) |
| Nathan Nolan | .... | S.H.I.E.L.D. Lieutenant (uncredited) |
| Richard Norris | .... | Hydra Soldier (uncredited) |
| Martin Poole | .... | Theatre Spectator (uncredited) |
| Christopher Poultney | .... | Times Square Pedestrian (uncredited) |
| Eric Reeve | .... | Reporter (uncredited) |
| Colin Reilly | .... | US Infantry Soldier (uncredited) |
| Nathan Robinson | .... | Lab Tech (uncredited) |
| Geoff Rolph | .... | Soldier (uncredited) |
| Shane Salter | .... | Hydra / Military Police (uncredited) |
| Geoff Searle | .... | US Marine (uncredited) |
| Drew Sherman | .... | HYDRA Soldier (uncredited) |
| Colin Stinton | .... | New York Taxi Driver (uncredited) |
| Michael Swan | .... | Dodgers Announcer (uncredited, Stimme) |
| Jayme Swiftt | .... | Soldier (uncredited) |
| Shaun Troke | .... | Prisoner of War (uncredited) |
| Sy Turner | .... | Hydra Soldier (uncredited) |
| Matt Tyzack | .... | Scientist (uncredited) |
| Chris Wilson | .... | American Civilian 1940s (uncredited) |