| Year | Film | Role | Notes |
| 1932 | This Is the Night | Stephen | With Lili Damita, Charles Ruggles, and Thelma Todd |
| Sinners in the Sun | Ridgeway | With Carole Lombard and Chester Morris |
| Singapore Sue | First Sailor | Musical Comedy short subject |
| Merrily We Go to Hell | Charlie Baxter | UK title: Merrily We Go to _____ With Sylvia Sidney and Fredric March |
| Devil and the Deep | Lieutenant Jaeckel | With Tallulah Bankhead and Gary Cooper |
| Blonde Venus | Nick Townsend | With Marlene Dietrich |
| Hot Saturday | Romer Sheffield | With Nancy Carroll and Edward Woods |
| Madame Butterfly | Lieutenant B.F. Pinkerton | With Sylvia Sidney and Charles Ruggles |
| 1933 | She Done Him Wrong | Capt. Cummings | With Mae West and Noah Beery, Sr. |
| The Woman Accused | Jeffrey Baxter | With Nancy Carroll |
| The Eagle and the Hawk | Henry Crocker | With Fredric March and Carole Lombard |
| Gambling Ship | Ace Corbin | With Jack La Rue and Glenda Farrell |
| I'm No Angel | Jack Clayton | With Mae West |
| Alice in Wonderland | The Mock Turtle | With W. C. Fields and Gary Cooper |
| 1934 | Thirty Day Princess | Porter Madison III | With Sylvia Sidney and Edward Arnold |
| Born to Be Bad | Malcolm Trevor | With Loretta Young (Heavily censored by the Hayes Office) |
| Kiss and Make-Up | Dr. Maurice Lamar | With Helen Mack and the WAMPAS Baby Stars of 1934 |
| Ladies Should Listen | Julian De Lussac | With Francis Drake and Edward Everett Horton |
| 1935 | Enter Madame | Gerald Fitzgerald | With top-billed Elissa Landi |
| Wings in the Dark | Ken Gordon | With Myrna Loy |
| The Last Outpost | Michael Andrews | With Claude Rains |
| Sylvia Scarlett | Jimmy Monkley | Directed by George Cukor With Katharine Hepburn |
| 1936 | Big Brown Eyes | Det. Sgt. Danny Barr | With Joan Bennett and Walter Pidgeon |
| Suzy | Andre | With Jean Harlow and Franchot Tone |
| The Amazing Quest of Ernest Bliss | Ernest Bliss | US title: Romance and Riches Alt title: The Amazing Adventure |
| Wedding Present | Charlie | With Joan Bennett |
| 1937 | When You're in Love | Jimmy Hudson | UK title: For You Alone With Grace Moore |
| Topper | George Kerby | With Constance Bennett |
| The Toast of New York | Nicholas "Nick" Boyd | With Edward Arnold and Jack Oakie |
| The Awful Truth | Jerry Warriner | Directed by Leo McCarey
With Irene Dunne
Introduced the "Cary Grant persona" |
| 1938 | Bringing up Baby | Dr. David Huxley | Directed by Howard Hawks
With Katharine Hepburn and Charles Ruggles |
| Holiday | John "Johnny" Case | Directed by George Cukor
With Katharine Hepburn
UK title: Free to Live |
| 1939 | Gunga Din | Sgt. Archibald Cutter | Directed by George Stevens
With Victor McLaglen and Douglas Fairbanks, Jr. |
| Only Angels Have Wings | Geoff Carter | Directed by Howard Hawks
With Jean Arthur, Thomas Mitchell, and Rita Hayworth |
| In Name Only | Alec Walker | With Carole Lombard and Charles Coburn |
| 1940 | His Girl Friday | Walter Burns | Directed by Howard Hawks
Remake of The Front Page
With Rosalind Russell |
| My Favorite Wife | Nick | Co-written by Leo McCarey
Directed by Garson Kanin
With Irene Dunne and Gail Patrick |
| The Howards of Virginia | Matt Howard | UK title: The Tree of Liberty
With Martha Scott |
| The Philadelphia Story | C.K. Dexter Haven | With Katharine Hepburn and James Stewart |
| 1941 | Penny Serenade | Roger Adams | Nominated – Academy Award for Best Actor
Directed by George Stevens
With Irene Dunne and Edgar Buchanan |
| Suspicion | Johnnie | Directed by Alfred Hitchcock
With Joan Fontaine |
| 1942 | The Talk of the Town | Leopold Dilg aka Joseph | With Ronald Colman and Jean Arthur |
| Once Upon a Honeymoon | Patrick "Pat" O'Toole | Directed by Leo McCarey
With Ginger Rogers |
| 1943 | Mr. Lucky | Joe Adams/Joe Bascopolous | With Laraine Day and Charles Bickford |
| Destination Tokyo | Capt. Cassidy | With John Garfield and Dane Clark |
| 1944 | Once Upon a Time | Jerry Flynn | With Janet Blair |
| Arsenic and Old Lace | Mortimer Brewster | With Priscilla Lane and Peter Lorre |
| None But the Lonely Heart | Ernie Mott | Nominated – Academy Award for Best Actor Written and directed by Clifford Odets
With Ethel Barrymore |
| 1946 | Without Reservations | Himself (cameo) | With Claudette Colbert and John Wayne |
| Night and Day | Cole Porter | Directed by Michael Curtiz |
| Notorious | T.R. Devlin | Directed by Alfred Hitchcock
With Ingrid Bergman and Claude Rains |
| 1947 | The Bachelor and the Bobby-Soxer | Dick | UK title: Bachelor Knight With Myrna Loy and Shirley Temple |
| The Bishop's Wife | Dudley | With Loretta Young and David Niven |
| 1948 | Mr. Blandings Builds His Dream House | Jim Blandings | With Myrna Loy and Melvyn Douglas |
| Every Girl Should Be Married | Dr. Madison W. Brown | With Betsy Drake |
| 1949 | I Was a Male War Bride | Capt. Henri Rochard | UK title: You Can't Sleep Here
With Ann Sheridan |
| 1950 | Crisis | Dr. Eugene Norland Ferguson | With Jose Ferrer |
| 1951 | People Will Talk | Dr. Noah Praetorius | With Jeanne Crain |
| 1952 | Room for One More | George "Poppy" Rose | With Betsy Drake |
| Monkey Business | Dr. Barnaby Fulton | Directed by Howard Hawks
With Ginger Rogers and Marilyn Monroe |
| 1953 | Dream Wife | Clemson Reade | With Deborah Kerr and Walter Pidgeon |
| 1955 | To Catch a Thief | John Robie | Directed by Alfred Hitchcock
With Grace Kelly |
| 1957 | The Pride and the Passion | Anthony | With Frank Sinatra and Sophia Loren |
| An Affair to Remember | Nickie Ferrante | A same-script remake of Love Affair (1939 film), both directed by Leo McCarey With Deborah Kerr |
| Kiss Them for Me | Cmdr. Andy Crewson | Directed by Stanley Donen
With Jayne Mansfield and Suzy Parker |
| 1958 | Indiscreet | Philip Adams | Nominated – Golden Globe Award for Best Actor – Motion Picture Musical or Comedy
Directed by Stanley Donen
With Ingrid Bergman |
| Houseboat | Tom Winters | With Sophia Loren |
| 1959 | North by Northwest | Roger O. Thornhill | Directed by Alfred Hitchcock With Eva Marie Saint, James Mason, and Martin Landau |
| Operation Petticoat | Lt. Cmdr. Matt T. Sherman | Nominated – Golden Globe Award for Best Actor – Motion Picture Musical or Comedy
With Dina Merrill and Arthur O'Connell |
| 1960 | The Grass Is Greener | Victor Rhyall, Earl | Nominated – Golden Globe Award for Best Actor – Motion Picture Musical or Comedy Directed by Stanley Donen
With Deborah Kerr, Robert Mitchum, and Jean Simmons |
| 1962 | That Touch of Mink | Philip Shayne | Nominated – Golden Globe Award for Best Actor – Motion Picture Musical or Comedy
Directed by Delbert Mann
With Doris Day and Gig Young |
| 1963 | Charade | Peter Joshua / Carson Dyle / Alexander Dyle / Adam Canfield / Brian Cruikshank | Nominated – BAFTA Award for Best Foreign Actor
Nominated – Golden Globe Award for Best Actor – Motion Picture Musical or Comedy
Directed by Stanley Donen
With Audrey Hepburn, Walter Matthau, and James Coburn |
| 1964 | Father Goose | Walter Christopher Eckland | Directed by Ralph Nelson
With Leslie Caron and Trevor Howard |
| 1966 | Walk, Don't Run | Sir William Rutland | With Samantha Eggar Remake of The More the Merrier
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