Chris Evans as Steve Rogers / Captain America

Samuel L. Jackson as Nick Fury

Scarlett Johansson as Natasha Romanoff / Black Widow

Robert Redford as Alexander Pierce

Sebastian Stan as Bucky Barnes / Winter Soldier

Anthony Mackie as Sam Wilson / Falcon

Cobie Smulders as Maria Hill

Frank Grillo as Brock Rumlow

Maximiliano Hernández as Jasper Sitwell

Emily VanCamp as Kate / Agent 13

Hayley Atwell as Peggy Carter

Toby Jones as Dr. Arnim Zola

Stan Lee as Smithsonian Guard

Callan Mulvey as Jack Rollins

Jenny Agutter as Councilwoman Hawley

Bernard White as Councilman Singh

Alan Dale as Councilman Rockwell

Chin Han as Councilman Yen

Garry Shandling as Senator Stern

Georges St-Pierre as Georges Batroc

Salvator Xuereb as French Pirate #1

Brian Duffy as French Pirate #2

Zack Duhame as Engine Pirate

Adetokumboh M'Cormack as French Radio Pirate

Christopher George Sarris as Skinny Steve

Aaron Himelstein as Launch Tech #1

Allan Chanes as Launch Tech #2

Joe Russo as Dr. Fine

Christopher Markus as SHIELD Interrogator #1

Stephen McFeely as SHIELD Interrogator #2

Pat Healy as Scientist #1

Ed Brubaker as Scientist #2

D.C. Pierson as Apple Employee

Danny Pudi as Com Tech #1

Bernie Zilinskas as Com Tech #2

Branka Katić as Renata

Angela Russo-Otstot as Garcia

Jon Sklaroff as Charlie XO

Chad Todhunter as Charlie Weapons Tech

Abigail Marlowe as SHIELD Tech

Jeremy Maxwell as Lead SHIELD Pilot

Emerson Brooks as Senior SHIELD Agent

Evan Parke as SHIELD Agent

Ricardo Chacon as Strike SGT. #1

Griffin M. Allen as Strike SGT. #2

Ann Russo as Strike Agent

Joe Rosalina as Strike Agent

Michael Debeljak as Strike Agent

Eddie J. Fernandez as Strike Agent

Jody Hart as 25ᵗʰ Floor Strike Agent

Steven Culp as Scudder

Derek Hughes as Human Resources Executive

Wendy Hoopes as Doctor

Ethan Rains as Lead EMT

Dominic Rains as CIA Instructor

Charles Wittman as Capitol Hill Police

Andy Martinez, Jr. as Capitol Hill Police

Michael De Geus as FBI Agent

Terence O'Rourke as FBI Agent

Anne Grimenstein as Committee Member

Dante Rosalina as Little Boy in the Smithsonian

Robert Clotworthy as Fury Car Voice (voice)

June Christopher as SHIELD Computer (voice)

Gary Sinise as The Smithsonian Narrator (voice)

Henry Goodman as Dr. List (uncredited)

Dean Barlage as SHIELD Agent (uncredited)

Joel Thingvall as Museum Visitor (uncredited)

Thomas Kretschmann as Baron Wolfgang von Strucker (uncredited)

Elizabeth Olsen as Wanda Maximoff / Scarlet Witch (uncredited)

Nestor Serrano as Committee General (uncredited)

Aaron Taylor-Johnson as Pietro Maximoff / Quicksilver (uncredited)

Joss Whedon as Man on Escalator in Museum (uncredited)

James Lewis as Smithsonian Museum Visitor