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| Audrey Hepburn | Sister Luke (Gabrielle van der Mal) |
| Peter Finch | Dr. Fortunati |
| Edith Evans | Rev. Mother Emmanuel (Belgium) |
| Peggy Ashcroft | Mother Mathilde (Africa) |
| Dean Jagger | Dr. Van Der Mal |
| Mildred Dunnock | Sister Margharita (Mistress of Postulants) |
| Beatrice Straight | Mother Christophe (Sanatorium) |
| Patricia Collinge | Sister William (convent teacher) |
| Eva Kotthaus | Sister Marie (Sanatorium) |
| Ruth White | Mother Marcella (School of Medicine) |
| Niall MacGinnis | Father Vermeuhlen (Leprosarium) |
| Patricia Bosworth | Simone (postulant who changed her mind) |
| Barbara O'Neil | Mother Didyma (War-time Hospital) |
| Lionel Jeffries | Dr. Goovaerts (School of Tropical Medicine) |
| Rosalie Crutchley | Sister Eleanor |
| Colleen Dewhurst | Archangel Gabriel (Sanatorium) |
Willful and outspoken Gabrielle van der Mal, the daughter of a prominent Belgian surgeon, leaves her upper-class existence to become a nun. As Sister Luke, she is eventually sent to the Belgian Congo, where she excels as a nurse working with a skilled doctor . However, her willingness to continue as a nun is challenged when her father is killed by the Nazis, and she no longer feels that she can maintain the neutrality of her order.
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