Chris Evans Steve Rogers / Captain America Scarlett Johansson Natasha Romanoff / Black Widow Sebastian Stan James 'Bucky' Barnes / Winter Soldier Anthony Mackie Sam Wilson / Falcon Cobie Smulders Maria Hill Frank Grillo Brock Rumlow Emily VanCamp Sharon Carter Hayley Atwell Peggy Carter Robert Redford Alexander Pierce Samuel L. Jackson Nick Fury Toby Jones Dr. Arnim Zola Jenny Agutter Councilwoman Hawley Maximiliano Hernández Jasper Sitwell Georges St-Pierre Georges Batroc Callan Mulvey Jack Rollins Alan Dale Councilman Rockwell Chin Han Councilman Yen Bernard White Councilman Singh Garry Shandling Senator Stern Danny Pudi S.H.I.E.L.D. Technician #1 Gary Sinise Smithsonian Narrator (voice) Stan Lee Smithsonian Guard Ed Brubaker Scientist #2 Joe Russo Dr. Fine Christopher Markus SHIELD Interrogator #1 Stephen McFeely SHIELD Interrogator #2 Salvator Xuereb French Pirate #1 Brian Duffy French Pirate #2 Zack Duhame Engine Pirate Adetokumboh M'Cormack French Radio Pirate Aaron Himelstein Specialist Cameron Klein Pat Healy Scientist #1 Branka Katić Renata Jon Sklaroff Charlie XO Abigail Marlowe SHIELD Tech Jeremy Maxwell Lead SHIELD Pilot Emerson Brooks Senior SHIELD Agent Evan Parke SHIELD Agent Ricardo Chacon Strike SGT. #1 Ann Russo Strike Agent Eddie J. Fernandez Strike Agent Jody Hart 25th Floor Strike Agent Robert Clotworthy Fury Car Voice (voice) June Christopher SHIELD Computer (voice) Henry Goodman Dr. List (uncredited) Thomas Kretschmann Baron Wolfgang von Strucker (uncredited) Elizabeth Olsen Wanda Maximoff / Scarlet Witch (uncredited) Nestor Serrano Committee General (uncredited) Aaron Taylor-Johnson Pietro Maximoff / Quicksilver (uncredited)