Michael G Wilson and Barbara Broccoli, producers of the Bond series, said in a statement: "We are so sad to learn that Eunice Gayson, our very first 'Bond girl', who played Sylvia Trench in Dr No and From Russia With Love, has passed away.
"Our sincere thoughts are with her family."
Gayson will go down in cinema history for helping coin Bond's catchphrase.
In the 1962 Dr No, Gayson's character Sylvia Trench is seen playing poker at the Le Cercle club.
After losing a few hands she suggests raising the stakes, to which Bond replies: "I admire your courage, Miss, er?"
She says: "Trench, Sylvia Trench. I admire your luck, Mr..."
Sean Connery then delivers the famous line: "Bond, James Bond."
Gayson was born in Surrey in 1928. She landed a number of on screen roles before and after her part in Bond.
She was cast in Hammer Horror's 1958 movie The Revenge of Frankenstein and appeared in several classic TV series such as The Saint and The Avengers.