McCann was known to a generation of children who grew up watching his children's shows in the New York City metropolitan area during the 1960s, having worked his way up to regional star status by apprenticing on a number of other children's shows, such as Captain Kangaroo and Rootie Kazootie (the show on which he met his one-time puppeteer and sidekick, Paul Ashley). The best-selling The First Family, an early '60s LP record album which lampooned the newly elected President John F. Kennedy and his family, included McCann among its voices.
Until late 1967, McCann hosted comedy/variety TV puppet shows in the New York area. McCann (with Ashley) did The Puppet Hotel for WNTA-TV, Channel 13; then Laurel & Hardy & Chuck, Let's Have Fun, and The Chuck McCann Show for WPIX, Channel 11; and finally, The Chuck McCann Show, The Great Bombo's Magic Cartoon Circus Lunchtime Show, and Chuck McCann's Laurel and Hardy Show for WNEW-TV, Channel 5. In addition, Chuck was the comedy sidekick on the WPIX long-running Clay Cole Show.
His career was burgeoning by the time he left Channel 5, a victim of changing TV trends. By the end of the 1960s, he had appeared to critical acclaim in the 1968 film The Heart Is a Lonely Hunter and performed regularly on CBS's The Garry Moore Show.
He began an animation acting career, doing everything from Bob Kane's Cool McCool to Sonny the Cuckoo Bird ("I'm cuckoo for Cocoa Puffs!") in commercials for General Mills. He had even been one of the stars of Turn-On, producer George Schlatter's ill-fated offshoot of Laugh-In.
In the 1970s, McCann's life and career shifted west, and he relocated to Los Angeles. He made frequent guest appearances on network television shows including Little House on the Prairie, Bonanza, Columbo, The Rockford Files and The Bob Newhart Show. He appeared in the 1973 made-for-TV movie The Girl Most Likely to... and was a regular on Norman Lear's All That Glitters.
In addition, he co-starred with Bob Denver in CBS's Saturday-morning sitcom Far Out Space Nuts, which he co-created. The 1970s also brought him fame in a long-running series of commercials for Right Guard antiperspirant: he was the enthusiastic neighbor with the catch phrase "Hi, guy!" who appeared on the other side of a shared medicine cabinet, opposite actor Bill Fiore.
McCann impersonated Oliver Hardy in commercials for various products (teaming with Jim MacGeorge as Stan Laurel), and for a few years, he played the holiday-season recurring role of Kris Kringle on the NBC soap opera Santa Barbara In 1965, he and John McCabe, were part of the founding four members of the now worldwide society of The Sons of the Desert, an appreciation club to the works of Laurel and Hardy. He also had a role in Kojak in 1974, under the name Charles McCann.
After The Heart Is a Lonely Hunter, McCann's motion picture career took a turn back into comedy with many supporting roles and a co-starring turn (with Tim Conway) in They Went That-A-Way & That-A-Way (1978). His most notable post-Hunter films were The Projectionist (1971), Jennifer on My Mind (1971), Linda Lovelace for President (1975), Foul Play (1978), C.H.O.M.P.S. (1979), The Comeback Trail (1982), Hamburger: The Motion Picture (1986), and Herbie Rides Again (1974), where he played Loostgarten, president of Loostgarten Wrecking Company. He also had a supporting role in the 1988 horror film Cameron's Closet. He had a brief appearance in Mel Brooks' 1993 comedy film Robin Hood: Men in Tights as a villager and also appeared as an innkeeper in another Brooks production; Dracula: Dead and Loving It in 1995.
In 1980, McCann and Paul Ashley were reunited for a pair of TV show pilots:Tiny TV (a satirical/variety puppet series aimed at adults for the cable market)
LBS Children's Theater (a children film anthology show where McCann and the Paul Ashley Puppets were to introduce reruns of primetime animated TV specials and theatrical cartoons from Europe). However, Paul Ashley was forced to leave the projects when he found to be suffering from Alzheimer's disease. Tiny TV never reached fruition, but LBS Children's Theater was picked up for national syndication in 1983. McCann emceed the series alone because Ashley did not live long enough to see the show, having died on September 3, 1984.
McCann voiced Dreamfinder in Disney's attraction Journey Into Imagination.
In the 1980s, McCann reprised a number of his best sketches from his New York television days as interstitial material for a two-hour presentation of cartoons on KCOP-TV, Channel 13 in Los Angeles. (He was assisted by Bob Ridgely.)
And in 1989, McCann returned to daily children's television one more time with Chuck McCann's Funstuff (produced by fellow New York kid show legend Sonny Fox). Chuck McCann's Funstuff was seen weekday mornings on KHJ (KCAL) from Monday, September 18, 1989 until Friday, October 13, 1989.
In the 1990s, McCann co-founded and participated in Yarmy's Army, a group of comedians and character actors of his generation who gathered regularly to cheer up Don Adams' brother Dick Yarmy, who was dying of cancer. A group with a massive array of comic talent, its members included Harvey Korman, Shelley Berman, Tim Conway, and many others.
After Yarmy's death, the group stayed together to cheer themselves up since increasing age and health problems made it increasingly more difficult for them to get steady work. In addition to having monthly dinners, they performed in various group-directed shows in select venues around the country.
McCann continued voice work for cartoons, playing Jollo, Bookworm, Bump-On-A-Log, and Woof in 1992's King's Quest VI: Heir Today, Gone Tomorrow. One of his best-known voiceover roles was The Thing in the Fantastic Four and Hulk animated series, as well as the villain Blizzard in another animated adaptation, Iron Man.
He also played Heff Heffalump, a recurring not-so-villainous character in Disney's The New Adventures of Winnie The Pooh. He was also the voice of Leatherneck on the second season of G.I. Joe. Throughout the 1990s and into the new millennium, he has been in commercials at Christmas time, he has played Santa Claus for one product or another—and TV/movie gigs (Sabrina, the Teenage Witch).
In the 2000s, McCann appeared in They Call Him Sasquatch (2003) and Dorf da Bingo King (with his old pal, Tim Conway). He has supplied voices for The Powerpuff Girls and Mickey's Twice Upon a Christmas. And he also moved into the field of video games, providing voices for True Crime: New York City.
McCann made an appearance in The Aristocrats (2005), with an animated rendition of a "clean" version of the "dirty" joke that serves as the movie's subject.
In 2006-07 he made appearances on The Radio Adventures of Dr. Floyd as Benjamin Franklin and Dr. Floyd's father. He has also made multiple appearances as a judge on Boston Legal, including the two-hour series finale in December 2008. In 2007, McCann played the villain Dalton Kern on the radio drama Adventures in Odyssey and also Navarro and Buck in Random! Cartoons.
In 2013, McCann voiced Moseph "Moe" Mastro Giovanni on an episode of Adventure Time, Mayor Grafton on The Garfield Show, and reprised Duckworth in DuckTales Remastered. In 2016, he reprised the role of the Amoeba Boys in the 2016 reboot of The Powerpuff Girls.
McCann was born in Brooklyn, New York, to a bandleader/singer father. McCann is a close friend of Hugh Hefner and a regular at the Playboy Mansion. During the 1980s, McCann appeared as an announcer in various Playboy videos, including Playboy Playmate Playoffs.