Chris Evans character Steve Rogers / Captain America
Scarlett Johansson character Natasha Romanoff / Black Widow
Sebastian Stan character Bucky Barnes / Winter Soldier
Anthony Mackie character Sam Wilson / Falcon
Cobie Smulders character Maria Hill
Frank Grillo character Brock Rumlow
Emily VanCamp character Sharon Carter
Hayley Atwell character Peggy Carter
Robert Redford character Alexander Pierce
Samuel L. Jackson character Nick Fury
Toby Jones character Dr. Arnim Zola
Maximiliano Hernández character Jasper Sitwell
Garry Shandling character Senator Stern
Georges St-Pierre character Georges Batroc
Callan Mulvey character Jack Rollins
Ng Chin Han character Councilman Yen
Jenny Agutter character Councilwoman Hawley
Alan Dale character Councilman Rockwell
Bernard White character Councilman Singh
Danny Pudi character S.H.I.E.L.D. Technician #1
D.C. Pierson character Apple Store Employee
Gary Sinise character Smithsonian Narrator (voice)
Stan Lee character Smithsonian Guard
Ed Brubaker character Scientist #2
Joe Russo character Dr. Fine (as Gozie Agbo)
Christopher Markus character SHIELD Interrogator #1
Stephen McFeely character SHIELD Interrogator #2
Thomas Kretschmann character Baron Wolfgang von Strucker (uncredited)
Henry Goodman character Dr. List (uncredited)
Elizabeth Olsen character Scarlet Witch (uncredited)
Aaron Taylor-Johnson character Quicksilver (uncredited)
Salvator Xuereb character French Pirate #1
Brian Duffy character French Pirate #2
Zack Duhame character Engine Pirate
Adetokumboh M'Cormack character French Radio Pirate
Christopher George Sarris character Skinny Steve
Aaron Himelstein character Specialist Cameron Klein
Allan Chanes character Launch Tech
Pat Healy character Scientist #1
Bernie Zilinskas character S.H.I.E.L.D. Technician #2
Branka Katić character Renata
Angela Russo-Otstot character Garcia
Jon Sklaroff character Charlie XO
Chad Todhunter character Charlie Weapons Tech
Abigail Marlowe character SHIELD Tech
Jeremy Maxwell character Lead SHIELD Pilot
Emerson Brooks character Senior SHIELD Agent
Evan Parke character SHIELD Agent
Ricardo Chacon character Strike SGT. #1
Griffin M. Allen character Strike SGT. #2
Ann Russo character Strike Agent
Joe Rosalina character Strike Agent
Michael Debeljak character Strike Agent
Eddie J. Fernandez character Strike Agent
Jody Hart character 25th Floor Strike Agent
Steven Culp character Scudder
Derek Hughes character Human Resources Executive
Wendy Hoopes character Doctor
Ethan Rains character Lead EMT
Dominic Rains character CIA Instructor
Charles Wittman character Capitol Hill Police
Andy Martinez, Jr. character Capitol Hill Police
Michael De Geus character FBI Agent
Terence O'Rourke character FBI Agent
Dean Barlage character SHIELD Agent
Anne Grimenstein character Committee Member
Dante Rosalina character Little Boy in the Smithsonian
Robert Clotworthy character Fury Car Voice (voice)
June Christopher character SHIELD Computer (voice)
Nestor Serrano character Committee General (uncredited)