Sometimes, between the clicks of a shutter, a magical, enduring relationship can develop between photographer and subject. Such was the case with legendary LIFE photographer Alfred Eisenstaedt and the luminous Italian movie star Sophia Loren. And so, when presented with 19 gorgeous, never-before-published photos taken by her old friend, Loren is delighted to see them -- but not at all surprised. "Oh, he must have shot thousands of pictures that never came out, Eisie," Loren tells LIFE.com during a recent interview, fondly remembering her camera-toting "shadow." Indeed, Eisenstaedt (who died in 1995) photographed the stunning actress numerous times at the height of her fame in the 1960s and early '70s, shooting countless rolls of film. Here, in celebration of Loren -- the subject of a May 4 tribute hosted by the Academy of Motion Picture Arts and Sciences, nearly 50 years after she won the Oscar for Best Actress -- LIFE.com presents the best of Eisie's never-seen Sophia Loren photos, as well as her revealing comments on the intimate, special moments they illustrate.