Boothe's publicist says he died of natural causes at his home in Los Angeles Sunday.
Boothe was known for playing bad guys in many films, including "Tombstone," "Sin City" and "The Avengers."
He also had roles in TV shows like "Deadwood," "24" and "Marvel's Agents of S.H.I.E.L.D."
The veteran actor, who grew up on a Texas farm, won an Emmy award in 1980 for playing cult leader Jim Jones in the TV movie "Guyana Tragedy: The Story of Jim Jones."
Friends and family called him a devoted husband and father, and a great actor.
Reaction poured in from actors who had worked with Boothe over the years.
Beau Bridges tweeted the news and called him "a dear friend, great actor, devoted father and husband."
It's with great sadness that I mourn the passing of my friend Powers Boothe. A dear friend, great actor, devoted father & husband.— Beau Bridges (@MrBeauBridges) May 14, 2017
Lea Thompson, who was in the original "Red Dawn" with Boothe, called him "a gentleman and a great actor."
He also had memorable roles playing the ruthless saloon owner Cy Tolliver in "Deadwood," the gunman Curly Bill Brocius in "Tombstone" and the corrupt senator in "Sin City."
Met him on Tombstone & married him in True Women. Powers Boothe was a wonderful actor & even better man. Sad month for cowboys. pic.twitter.com/tiQnMqFJjP— Dana Delany (@DanaDelany) May 15, 2017
Terrible. We were incredibly lucky to have him on Shield. He taught me a lot. RIP Powers. My heart is with his family.— Chloe Bennet (@ChloeBennet4) May 15, 2017
A private service will be held in Texas where he was from.
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The Associated Press contributed to this report.