Gorshin's wife of 48 years, Christina, was at his side when he died Tuesday at Providence Saint Joseph Medical Center, his agent and longtime friend, Fred Wostbrock, said Wednesday.
"He put up a valiant fight with lung cancer, emphysema and pneumonia," Mrs. Gorshin said in a statement.
Despite dozens of TV and movie credits, Gorshin will be forever remembered for his role as the Riddler, Adam West's villainous foil in the question mark-pocked green suit and bowler hat on "Batman" from 1966 to 1969.
The Riddler's high-pitched laugh was based on his own, Gorshin told AP Radio in 1997. "I fooled around with all kinds of different laughs and then I found out that when I do laugh I get this high-pitched laugh and I thought, 'This is what I'm going to use.'"
"It really was a catalyst for me," Gorshin recalled in a 2002 Associated Press interview. "I was nobody. I had done some guest shots here and there. But after I did that, I became a headliner in Vegas, so I can't put it down."
West said the death of his longtime friend was a big loss.
"Frank will be missed," West said in a statement. "He was a friend and fascinating character."
In 2002, Gorshin portrayed George Burns on Broadway in the one-man show "Say Goodnight Gracie." He used only a little makeup and no prosthetics.
"I don't know how to explain it. It just comes," he said. "I wish I could say, `This is step A, B and C.' But I can't do that. I do it, you know. The ironic thing is I've done impressions all my life -- I never did George Burns."
Gorshin's final performance will be broadcast on Thursday's CBS series "CSI: Crime Scene Investigation."
Later, he took his impressions to "The Ed Sullivan Show" on a memorable evening -- the same night the Beatles were featured.
When asked by the AP how it felt to be the unlucky performer following the Beatles, he said, "I looked out the window of my dressing room and said, 'Look at all the kids that came to see me!'"
He also did impressions in Las Vegas showrooms, opening for Darin and paving the way for other impressionists like Rich Little. Sammy Davis Jr. said it was Gorshin who taught him to do impressions, Wostbrock said.
"He said you had to look like them and walk like them. Once you get that down, the voice comes easy," he said.
Gorshin's movie roles included "Bells are Ringing" (1960) with his idol Dean Martin and a batch of fun B-movies such as "Hot Rod Girl" (1956), "Dragstrip Girl" (1957) and "Invasion of the Saucer Men" (1957).
"He was fun, fascinating, wild and always a class act," Wostbrock said. "Here's a guy who always wore great clothes, stood up when a woman walked into the room -- he was a gentleman. We did all our deals with a handshake. There was never a signed contract."
His other TV credits included roles on "General Hospital, "The Edge of Night" and "The Munsters" as well as guest appearances on "Donny & Marie," "The Tonight Show Starring Johnny Carson," "Late Night with Conan O'Brien," "Lois & Clark: The New Adventures of Superman," "Murder, She Wrote," "The Fall Guy," "Buck Rogers in the 25th Century," "Wonder Woman," "Charlie's Angels" and "Police Woman."
Wostbrock said the funeral would be private and Gorshin would be buried in the family plot in Pittsburgh.