At nearly every stage of Natalie Wood's career — the early days as a cute studio-contract moppet; her teenage Method experiments inspired by her work in Rebel Without a Cause; and her emergence as a powerful leading lady who could more than hold her own with Warren Beatty and Steve McQueen — LIFE's photographers were there, capturing Wood's talent and beauty as they blossomed over the years.
But not every picture from those many rolls of film could make it to print, of course. Here, LIFE.com presents a selection of the best photos of the late, radiant star which were not originally published in LIFE magazine.
Natalie Wood died, far too young, in 1981. She was just 43 years old. She drowned near Santa Catalina Island, off the coast of California. In 2012, the Los Angeles County Medical Examiner reclassified the cause of her death as "drowning and other undetermined factors."
Liz Ronk, who edited this gallery, is the Photo Editor for LIFE.com. Follow her on Twitter @lizabethronk.