In her early career, Wood usually played in films in which Natalie appeared. Starting in the 1960s, her own career took off. After appearing on the short-lived drama series The Long, Hot Summer, she landed the role of Sandy Webber on the soap series Peyton Place. She played the role from 1966–67. In 1970, Wood was approached by Hugh Hefner and asked to pose for Playboy to which she agreed. The Playboy pictures appeared in the April 1971 issue, along with Wood's poetry. She was cast as a Bond girl, Plenty O'Toole, in the James Bond film, Diamonds Are Forever (1971).