Her daughter called her "a blessing and the light of my life".
The New Jersey natives had three children.
Frank went on to Wednesday actress Mia Farrow and Barbara Marx before his fatal heart attack at the age of 82.
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Nancy Barbato and Frank Sinatra started dating when they were teens.
"My mother passed away peacefully tonight at the age of 101".
Two years later, the Sinatras separated after Frank's affair with Ava Gardner became public knowledge, with Frank marrying Gardner, the second of his four wives, shortly after.
Nancy Sinatra Senior was born as Nancy Barbato on March 25, 1917 and met Frank in 1934 at the New Jersey holiday resort of Long Branch. "Godspeed, Momma. Thank you for everything", she added. Nancy worked as a secretary while Frank worked as both a singer and a waiter. The couple had three children together as Frank rose to fame and fortune with his music.
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After their 1939 marriage, Frank and Nancy lived in an apartment in Jersey City, N.J., her hometown.
Attempts to reach representatives for Nancy Sinatra Jr. late Friday were unsuccessful. Weeks after the pair's divorce became final in 1951, Sinatra's ex-husband married Gardner, while Sinatra went on to raise the couple's three children: Nancy, Frank Jr. and Tina.
She never remarried, and devoted her life to charity and her family, her daughter said.
Sinatra divorced Gardner two years later, and went on to marry Mia Farrow and then Barbara Marx.
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Gay Talese, in 1966, wrote there was "no bitterness", and instead, only "great respect and affection" between Frank and Nancy.