She also starred in Mark Robson's feature film Limbo and received excellent reviews. It was a big feat for a young actress to have starred in just a few years in two major feature films and appeared in many TV films. She went on starring in various TV movies-of-the-week becoming a TV scream queen as she starred in many thrillers including titles such as Satan's School for Girls, Killer Bees where she co-starred with the Hollywood legend Gloria Swanson, Death Cruise, Death Scream, Death at Love House etc. Producers Aaron Spelling and Leonard Goldberg spotted Jackson and recruited her for the role of nurse Jill Danko on their new ABC police drama series, The Rookies. She played the role of Nurse Danko for 4 whole years. The audience loved her character and bombarded ABC with more letters than the rest of the cast received. And the big boom took place in 1976 when Aaron Spelling, producer of The Rookies signed Kate to co-star as Sabrina Duncan in Charlie's Angels. Charlie's Angels was actually the idea of Kate Jackson. She was discussing with Aaron Spelling at the 20th Century Fox Studios when she noticed a painting on the wall of three angels and the series developed from that.

The rest is almost television history. Kate Jackson along with her co-angels, Farrah Fawcett-Majors and Jaclyn Smith, became household names overnight and her careers zoomed sky-high. In 1977, Kate Jackson's first year on Charlie's Angels, she received the first of two Emmy nominations for Best Actress in a Dramatic Series. She was also nominated as Best Supporting Actress for the NBC series pilot James at 15. For 3 years she was Charlie's smartest angel, "the brainy one" and the only one who was a qualified actress. Kate Jackson continued to appear in various roles both on TV and cinema, including Thunder and Lightning produced by Roger Corman. In 1979 she married actor Andrew Stevens and after she wasn't allowed to star in the feature film Kramer Vs Kramer and Meryl Streep took the lead role in the landmark film “Kramer vs. Kramer,” – netting her an Oscar for Best Actress along the way – a disappointed Jackson, who had had dibs on the role initially, vowed never to lose an important role because of her light-weight TV commitment. She had also just married actor Andrew Stevens and had grown tired of the constant interest in her off-screen romantic life. After the finale of season three in the spring of 1979, Jackson took off her halo permanently – leaving “Charlie’s Angels” with no apparent leader. She left the show after acrimonious disagreements with the producers that ended in the comic, "I quit!" "You can't quit! You're fired!" routine.

Being unhappy on the Charlie's Angels set throughout the last season, she had described the show as a bit of fluff "so light it would take a week to get to the floor if you dropped it from the ceiling," so she wasn't exactly heartbroken to leave it behind. Perfume model Shelley Hack, who had little-to-no acting experience, stepped in as a brainy replacement for Bri – but Jackson was a hard component to replace. The show teetered on for another two seasons, before being cancelled in 1981. Her prospect was a quiet family life and a production company with her husband. They produced and stared in the TV remake of the classic Hollywood film Topper which also was the pilot for a TV series that was never made. But her marriage with young Andrew Stevens didn't survive and they divorced back in 1980.  Kate focused on her career again and starred in various TV films such as Thin Ice and Listen to your Heart and made the big step with 2 big screen films, one black comedy called Dirty Tricks that got very poor reviews and the controversial  Making Love, co-starring with Harry Hamlin and Michael Ontkean, a film that received excellent reviews. She married David Greenwald in 1982 and together they created the production company Shoot the moon. In 1983 she returned to television with the CBS spy-comedy series called Scarecrow and Mrs. King. In the show's pilot, Kate's character, a recently divorced housewife and mother, accidentally gets pulled into a web of espionage by square-jawed, big-armed hunk Bruce Boxleitner. Through several unlikely twists of fate, (Mrs.) Amanda King found herself working as a secret agent, building up sexual tension with her sexy colleague. Her own company owned and produced the series. The series lasted 4 whole years and the fans and critics loved it. Amanda King was a role full of challenges and completely different than that of Sabrina's in Charlie's Angels. Kate divorced Greenwald in 1984.

In January 1987, Jackson discovered a lump in her breast and underwent a lumpectomy. After the end of Scarecrow and Mrs. King in 1987, Kate decided to return to TV with a witty NBC series that was actually based on  Diane Keaton's 1987 film Baby Boom. Kate reprised Diane's role as J.C. Wiatt, a single, busy executive who finds herself an instant mom when she unexpectedly gets custody of a dead relative's infant daughter. The series lasted only for a few months as the audience didn't like it. In 1989 she starred in a comedy for the big screen called Loverboy. Yet her breast cancer returned and she had to undergo a partial mastectomy. Kate's successful battle with breast cancer made the cover of People magazine May 11, 1992. In the cover story, she recounted the life-changing experience. "I had to decide whether I wanted to live or to die," she said. "Once you choose life, as I did, it's never the same."