She had a recurring role from 2002 to 2004 in the drama series The District and appeared as Olivia Hodges in two episodes of CSI: Crime Scene Investigation in 2012.

[4] Smith's career aspirations shifted to modeling and acting as she found work in television commercials and print ads, including one for Listerine mouthwash.

Voiced by John Forsythe, the Charles Townsend character presented cases and dispensed advice via a speakerphone to his core team of three female employees, to whom he referred as "Angels".

The program earned a huge Nielsen rating, causing the network to air it a second time and confirm production for a series, with all of the principal characters with the exception of Stiers.

The show would become a big success not only in the U.S. but, in successive years, in syndication around the world, spawning a cottage industry of peripheral products, particularly in the show's first three seasons, including several series of bubble gum cards, two sets of fashion dolls, numerous posters, puzzles, and school supplies, novelizations of episodes, toy vans, and a board game, all featuring Smith's likeness.

Jackson departed at the end of the third season, and proved harder to replace, as first Shelley Hack and then Tanya Roberts were brought in to try re-igniting the chemistry, media attention and ratings success enjoyed by the earlier teams.

[7] Smith's first two acting ventures outside the Angels mold (as an actress of note) was the CBS-TV movie of the week Escape from Bogen County in 1977, and Season 1 Episode 2 of "The Love Boat" (aired October 1, 1977) where she played Janette Bradford cruising solo while being watched by the private eye her husband hired.

Following the cancellation of Charlie's Angels in 1981, Smith starred in the title role of the critically acclaimed television movie Jacqueline Bouvier Kennedy, earning her a Golden Globe nomination for Best Actress.

In 1983, Smith starred as Jennifer Parker in the TV movie Rage of Angels, based on the novel by Sidney Sheldon.

[8] Smith continued to appear in a number of television movies and miniseries during the 1980s and 1990s including George Washington, The Night They Saved Christmas (both 1984), Florence Nightingale (1985), Windmills of the Gods (1988) – another TV film based on a Sidney Sheldon novel – The Bourne Identity[9] (also 1988); adapted from author Robert Ludlum's novel of the same name; Settle the Score (1989), Lies Before Kisses, The Rape of Dr. Willis (both 1991), In the Arms of a Killer (1992), and several TV versions of Danielle Steel novels, including Kaleidoscope (1990) and Family Album (1994).

In 1989, she played the title role in Christine Cromwell, a mystery television series based in San Francisco, but which only lasted one season.

In August 2006, Smith reunited with her angels co-stars Farrah Fawcett and Kate Jackson at the 58th Primetime Emmy awards in tribute to producer Aaron Spelling who had died earlier that year.

[15] In March 2010, Smith returned to acting after a five-year absence with a guest role on the NBC television drama Law & Order: Special Victims Unit.

A season 15 episode of The Simpsons ("The Fat and the Furriest") lampooned Smith's many business successes, portraying her as having her own line of axe heads.

[18] Her foray into home furnishings was extended to Kmart stores in the fall of 2008, with the chain's introduction of its Jaclyn Smith Today product line of bedding and bath accessories.