Open-Door Policy

Ray shadowed Natalie on-and-off for about six weeks, and in that time he got to know the remarkably down-to-earth actress well. "She was so wonderful and not at all a diva," he recalls. "She was eager to help and work. She was just interested in being a part of that story." The intimate moments Ray captured, like this one of Natalie in bed with her dogs, speak to a confident, carefree woman with little pretense. In 1963 — before the marriage to producer Richard Gregson, before the second marriage to actor Robert Wagner — Natalie was just a single gal about town, living in a modest home in LA.

All in the Family

Natalie, who landed her first major film role in 1947's Miracle on 34th Street at the age of eight, owed her early success to a driven Russian mother, Maria (pictured far left). "She modeled Natalie on the Shirley Temple template... and it worked," says Ray of Natalie's mother. "[She] saved all kinds of pictures and had [Natalie's] baby shoes. Somewhere along the line, I took a picture of the mother holding the baby shoes." Conversely, Ray recalls Natalie's Ukrainian father Nick, a film prop maker, as quiet. (Also pictured: Natalie’s sister, Lana.)

Glamour Puss

At the time of the LIFE shoot, Natalie was filming the movie Sex and the Single Girl, inspired by the advice book by Helen Gurley Brown and co-starring Tony Curtis, Peter Fonda, and Lauren Bacall. Here, Natalie — dressed to the nines — rests against a contraption meant to keep her gown wrinkle-free. "Stars did that from the very beginning in Hollywood," explains Ray. "Once they got them all dressed just the way they liked, they didn’t want them to sit down." Sex and the Single Girl would become one of the top 10 grossing films of 1964.

Working Overtime

On breaks from filming, Ray would accompany Natalie on various errands around town, whether it be consulting with Sex and the Single Girl costume designer Edith Head (pictured here) or rubbing elbows with Hollywood super-producer Ray Stark, who worked on Wood’s 1961 film West Side Story. "I remember that so well because Ray Stark was standing in these lifts, and he still wasn’t very tall," says Ray. "I have white eyebrows and he just took one look at me and he said, 'You should get your eyebrows dyed.' I don’t know why a photographer needed dark eyebrows."

After Hours

Given her early entrée into Hollywood, it’s no surprise Natalie had a wide social circle in La La Land — one that included her Sex and the Single Girl co-star Tony Curtis, pictured here playing billiards with the actress. "Tony had a big party," Ray explains. "That’s when he was married to Janet Leigh and had a big house." The guest list also included Romanian-American actor Edward G. Robinson, whom Ray recalls Natalie chatting with in Russian.

Getting Physical

Today’s starlets hardly invented #fitspo. Even in the '60s, actresses like Natalie were working up a sweat at the gym — though some didn’t necessarily like having their picture taken while doing it. "[Oscar-winning actress] Jennifer Jones was in the same class, and when I started to pull out the light and photograph Natalie she just screamed out of there," Ray recalls with a laugh. "She was afraid I’d get her without makeup and everything."

Beach Babe

Innately confident due to her years in front of the camera (and maybe that regular gym routine), Natalie didn't shy from the more revealing moments of Ray's shoot. And obviously, he says, she was beautiful: "I mean, a sculptor would have gone crazy."

Rough Waters

Natalie was the consummate professional throughout Ray’s shoot, but he does recall one moment — eerily prescient — in which Natalie became visibly uncomfortable. "We took a boat ride to Catalina, which, when you think back on it now, is really something. The sea was kind of rough going over there, and nobody enjoyed the ride. And Natalie, in particular, didn’t like it and mentioned she couldn’t swim and didn’t like the water. I don’t think she liked boats, and how she ended up on a yacht drowning off of Catalina years later, I just have no idea. It didn’t make any sense," remembers Ray.

The Eyes Have It

But, ultimately, what Ray remembers most from his time with Natalie all those years ago was her ability to convey any emotion — be it wonder, joy, or sorrow — through her big doe eyes. "Her eyes would just melt your heart," recalls Ray.

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