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Deborah leaves Noodles because his life as a gangster is incompatible with her ambition to become a star, a fact she recognizes from childhood. She tells him he would 'lock her up and throw away the key' if she stayed. The final break occurs in 1933 when, after she announces she is leaving for Hollywood, Noodles rapes her in a limousine. The next morning, she symbolically shuts him out of her life by closing the window shade of her train as she departs.
Deborah Gelly leaves Noodles in Once Upon a Time in America for a combination of reasons stemming from her personal ambition, his criminal life, and a final, devastating act of violence committed by Noodles.
Here are the specific details:
From her youth, Deborah was intensely ambitious and aspired to become a famous dancer and actress, a goal which required her to leave the Jewish ghetto of the Lower East Side.
The definitive and immediate reason for their final break in the 1930s is a brutal act of violence committed by Noodles.
The summary omits the dynamic where Noodles repeatedly prioritizes his loyalty to Max and the gang over Deborah (e.g., 'Go on, Noodles, your mother's calling you'), which reinforces her belief that he will never change.