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According to Munro, her career took off in 1966 when her mother and photographer friend entered some headshots of her to Britain's Evening News (London) "Face of the Year" contest.
"I wanted to do art. Art was my love. I went to art school in Brighton but I was not very good at it. I just did not know what to do. I had a friend at the college who was studying photography and he needed somebody to photograph and he asked me. Unbeknownst to me, he sent the photographs to a big newspaper in London. The famous fashion photographer, David Bailey, was conducting a photo contest and my picture won."
This led to modelling chores, her first job being for Vogue magazine at the age of 17. She moved to London to pursue top modelling jobs and became a major cover girl for fashion and TV advertisements while there. Decorative bit parts came her way in such films as Casino Royale (1967) and Where's Jack? (1969). One of her many photo ads got her a screen test and a one-year contract at Paramount where she won the role of Richard Widmark's daughter in the comedy/western A Talent for Loving (film) (1969).
1969 proved to be a good year for Munro, because it was then that she began a lucrative 10-year relationship with Lamb's Navy Rum. Her image was plastered all over the country, and this would eventually lead to her next big break.
"The most challenging scenes involved lying in the coffin with Vincent," she reveals. "You see, I’m allergic to feathers and I was attired in this beautiful negligee – but it was covered with feathers! It took a great deal of willpower not to sneeze or sniffle. On occasion, I would simply have to sneeze and this would result in having to do another take."
She would reprise the role in the sequel, Dr. Phibes Rises Again in 1972. In the same year, she was referred to in Colin Blunstone's song "Caroline Goodbye", a song about the break-up of their relationship.
Hammer Films CEO, Sir James Carreras, spotted Munro on a Lamb's Navy Rum poster/billboard. He asked his right hand man, James Liggett, to find and screen test her. She was immediately signed to a one-year contract. Her first film for Hammer proved to be something of a turning point in her career. It was during the making of Dracula AD 1972 that she decided from this film onward she was a full-fledged actress. Up until then, she was always considered a model who did some acting on the side.
Munro completed her contract for Hammer with Captain Kronos – Vampire Hunter in 1974. Directed by Brian Clemens, she plays the barefoot gypsy girl Carla. In Paramount Pictures DVD commentary, Clemens explains that he envisioned the role as a fiery, Raquel Welch type, red-head. Hammer pushed for Munro, and the script was adapted accordingly.
Munro has the distinction of being the only actor ever signed to a long-term contract by Hammer Films. She would later turn down the lead female roles in Hammer's Dr. Jekyll and Sister Hyde, Frankenstein and the Monster from Hell, and the unmade Vampirella because they required nudity.Munro with Charles H. Schneer in 1974 in Amsterdam during the premiere of The Golden Voyage of SinbadMunro in Amsterdam in 1974
"I got the part – I had been signed by Hammer, for one year, for a contract, out of which I did two films, one being Dracula AD 1972, and the second one being Captain Kronos – Vampire Hunter, which, kind of, would come full-circle, to Sinbad. It was written and directed by Brian Clemens, who wrote the screenplay for The Golden Voyage of Sinbad, so, I was lucky enough to be chosen for Captain Kronos, and they were searching for somebody to do Sinbad, and they wanted a big name, somebody American, or well-known, but Brian said "No". He kept lobbying Charles Schneer [producer] and Ray Harryhausen — saying: 'I think you should come and look at the rushes, and see what you think, because I think she's right'. So, they said "No", but, eventually, Brian persuaded them to do that, and they saw the rushes, and that was how I got the part. So, it was lovely, like work-out-of-work. I was very lucky to have done that."
Other appearances during this time included I Don't Want to Be Born (1975) with Joan Collins, and At the Earth's Core (1976) with Peter Cushing and Doug McClure. She appeared also as Tammy, a nursing employee of a sinister health farm, in "The Angels of Death" (1977), an episode of the TV series The New Avengers that featured also rising stars Pamela Stephenson and Lindsay Duncan. This was notable, among other things, for a vicious fight between Munro and Joanna Lumley's Purdey.
In 1977, Munro turned down the opportunity to play villainess Ursa in Superman in favour of what would become her most celebrated film appearance, Naomi in The Spy Who Loved Me,who seductively winks at Bond while trying to gun him down from her helicopter. Cubby Broccoli urged Caroline to make her way to America in search of more lucrative offers. She declined, preferring to stay close to her family.
Munro continued to work in numerous British and European horror and science fiction films through the 1970s and 1980s, most notably Starcrash (1979) with David Hasselhoff,Christopher Plummer and Marjoe Gortner. Munro's dialogue was completely redubbed by another actress, even for English language prints of the film.
Munro's career continued to thrive well in the 1980s, appearing in many slasher and Eurotrash productions. Her first film shot on American soil was the William Lustig productionManiac (1980). This was soon followed by the "multi-award winning, shot during the Cannes Film Festival" shocker The Last Horror Film (1982) (directed by David Winters), in which she was reunited with her Maniac co-star Joe Spinell. She had a cameo role in the cult classic slasher Don't Open 'Til Christmas as a singer (1984), Slaughter High (1986), Paul Naschy's Howl of the Devil (1987), and Jess Franco's Faceless (1988), followed in rapid succession. She reteamed with Starcrash director, Luigi Cozzi, for Il Gatto nero in 1989, though this would be her last major film appearance.
Throughout the 1980s, Munro was often cited by the press as being a candidate for the co-starring role in a proposed (but never produced) feature film based upon Doctor Who. The feature was being co-produced by her second husband George Dugdale. At various times, press reports linked her with numerous actors touted to play the role of The Doctor.
In 1984, Munro signed a recording contract with Gary Numan's label Numa Records, and released a dance single called "Pump Me Up". Written and produced by Numan, the single hardly sold, and Numan admitted later that his label was probably to blame. His original version of the song can be found on his 1984 album Berserker. Munro and Numan had a brief affair in 1984, but because of the break-up, Numan cancelled plans to produce an album for her and dropped her (and her younger brother, Lee), from his label. Numan publicly trashed her as a greedy sexbomb bimbo, and she is the subject of his 1986 song "The Need" from his Strange Charm album.
Munro also provided vocals and lyrics for the song "Warrior of Love" which she sang in the film Don't Open Till Christmas. The song was never officially released, although it can be found easily on the internet.
Between 1984 and 1987, Munro was also a hostess on the Yorkshire Television game show 3-2-1. Munro was also a popular pin-up girl during this time, though she refused to pose nude. In the early 1980s, she appeared in music videos with Adam Ant and Meat Loaf.
By the early 1990s Munro decided to focus her efforts more on her children, Georgina and Iona, and her husband George. Her film roles were confined to performing cameos as herself in Night Owl (1993); as Mrs. Pignon in To Die For(1994); and as the counsellor in her friend Jeffrey Arsenault's film Domestic Strangers (1996).