In terms of her most technically impressive performance, I think she never topped her work as Sister Luke in THE NUN'S STORY. Her work there is so internal and understated, and she couldn't rely on glamor or charm to pull it off. It's the movie I always think of when people claim she had no talent. That final scene with her walking down the alley alone is really one for the ages.
But my personal favorite performance of hers is Susy Hendrix in WAIT UNTIL DARK. Aside from portraying blindness well, she does great juggling her character's vulnerability, bitterness, fear, and inner strength-- for me, that was one of her most fully realized performances, full stop, and it was my movie that made me a fan after years of not thinking much of her as an actress. It made me go back to her other movies to re-evaluate them.
So anyway, here's my list:
THE NUN'S STORY
WAIT UNTIL DARK
ROMAN HOLIDAY (her first big role and she is just amazing, especially with portraying Ann's gradual arc from frightened young woman to dutiful leader)
HOW TO STEAL A MILLION (the best of her comedic roles-- her timing and charm are fantastic)
BREAKFAST AT TIFFANY'S (I know some feel she was miscast, but I think her work is great here and despite it being her signature role, it is one of her least characteristic)
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