| Year | Title | Role | Director | Co-stars | Notes |
|---|
| 1929 | Bulldog Drummond | Capt. Hugh "Bulldog" Drummond | F. Richard Jones | Claud Allister, Joan Bennett, Montagu Love | Nominated – Academy Award for Best Actor |
| Condemned | Michel | Wesley Ruggles | Ann Harding, Louis Wolheim, Dudley Digges | Nominated – Academy Award for Best Actor |
| 1930 | Raffles | Raffles | George Fitzmaurice Harry d'Abbadie d'Arrast | Kay Francis, Frederick Kerr, Bramwell Fletcher, Frances Dade |
| The Devil to Pay! | Willie Hale | George Fitzmaurice | Loretta Young, Frederick Kerr, Myrna Loy |
| 1931 | The Unholy Garden | Barrington Hunt | George Fitzmaurice | Fay Wray, Warren Hymer |
| Arrowsmith | Dr. Martin Arrowsmith | John Ford | Helen Hayes, Richard Bennett, Myrna Loy |
| 1932 | Cynara | Jim Warlock | King Vidor | Kay Francis, Phyllis Barry, Henry Stephenson |
| 1933 | The Masquerader | Sir John Chilcote / John Loder | Richard Wallace | Elissa Landi |
| 1934 | Bulldog Drummond Strikes Back | Capt. Hugh "Bulldog" Drummond | Roy Del Ruth | Loretta Young, Warner Oland, Charles Butterworth, Una Merkel, C. Aubrey Smith |
| 1935 | Clive of India | Robert Clive | Richard Boleslawski | Loretta Young, Colin Clive |
| The Man Who Broke the Bank at Monte Carlo | Paul Gaillard | Stephen Roberts | Joan Bennett, Nigel Bruce, Colin Clive |
| A Tale of Two Cities | Sydney Carton | Jack Conway | Elizabeth Allan, Edna May Oliver, Reginald Owen, Basil Rathbone, Blanche Yurka |
| 1936 | Under Two Flags | Sgt. Victor | Frank Lloyd | Claudette Colbert, Victor McLaglen, Rosalind Russell |
| 1937 | Lost Horizon | Robert Conway | Frank Capra | Jane Wyatt, Edward Everett Horton, Thomas Mitchell, Margo, Isabel Jewell, H. B. Warner, Sam Jaffe | Seven minutes of film missing, though the soundtrack is intact. |
| The Prisoner of Zenda | Maj. Rudolf Rassendyll / King Rudolf V | John Cromwell | Madeleine Carroll, Douglas Fairbanks, Jr., C. Aubrey Smith, Raymond Massey, Mary Astor | Presented in sepiatone[15] |
| 1938 | If I Were King | François Villon | Frank Lloyd | Frances Dee, Basil Rathbone |
| 1939 | The Light That Failed | Dick Heldar | William Wellman | Walter Huston, Ida Lupino |
| 1940 | Lucky Partners | David Grant | Lewis Milestone | Ginger Rogers, Jack Carson |
| 1941 | My Life with Caroline | Anthony Mason | Lewis Milestone | Anna Lee, Charles Winninger |
| 1942 | The Talk of the Town | Professor Michael Lightcap | George Stevens | Cary Grant, Jean Arthur, Edgar Buchanan, Glenda Farrell |
| Random Harvest | Charles Rainier | Mervyn LeRoy | Greer Garson, Philip Dorn, Susan Peters | Nominated — Academy Award for Best Actor Nominated — New York Film Critics Circle Award for Best Actor |
| 1944 | Kismet | Hafiz | William Dieterle | Marlene Dietrich, James Craig, Edward Arnold, Joy Ann Page | Technicolor |
| 1947 | The Late George Apley | George Apley | Joseph L. Mankiewicz | Peggy Cummins, Edna Best |
| A Double Life | Anthony John | George Cukor | Signe Hasso, Edmond O'Brien, Shelley Winters | Academy Award for Best Actor Golden Globe Award for Best Actor |
| 1950 | Champagne for Caesar | Beauregard Bottomley | Richard Whorf | Celeste Holm, Vincent Price, Barbara Britton, Art Linkletter |
| 1956 | Around the World in 80 Days | Great Indian Peninsular Railway Official | Michael Anderson | David Niven, Cantinflas, Shirley MacLaine, Robert Newton | Todd-AO EastmanColor |
| 1957 | The Story of Mankind | The Spirit of Man | Irwin Allen | Vincent Price, Cedric Hardwicke | Technicolor, (final film role) |