More than 50 years ago, on October 18, 1961, Natalie Wood premiered one of her most iconic movie roles: Maria, the 20th-century twist on Shakespeare’s tragically lovelorn Juliet, in the big-screen version of West Side Story. That Wood could nail the tricky mix of effervescence and anguish the part required was no surprise — after all, at just 23 years old, she was already a Hollywood veteran, an Oscar-nominated star whose astonishing talent had been honed since the age of 4.

And at nearly every stage of her career — the early days as a cute studio-contract moppet; her teenage Method experiments inspired by her work in Rebel Without a Cause; her emergence as a powerful leading lady wooing Warren Beatty and Steve McQueen onscreen — LIFE’s photographers were there, capturing Wood’s talent and beauty as they blossomed over the years.

Not all those pictures 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 — pictures that were not originally published in the magazine.

NOTE: This story and some of the images in the gallery originally appeared, in substantially different form, on an earlier incarnation of LIFE.com.