The actor died in his sleep of natural causes at his home here, his representative confirmed to The Hollywood Reporter.
Boothe, who grew up in Texas, had done both character and villainous roles in his career spanning almost half a century.
Initially, he featured in a number of Shakespearean productions including Henry IV and made his Broadway debut in the late '70s in "Lone Star & Pvt. Wars".
In 1980, Boothe won an Emmy for lead actor in a limited series or special for playing cult leader Jim Jones in "Guyana Tragedy: The Story of Jim Jones".
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Out of his recent outings, Boothe played the role of Gideon Malick as part of the Marvel Cinematic Universe, debuting the role in 2012's "The Avengers" and reprising it on ABC's "Agents of S.H.I.E.L.D".
He also appeared on TV shows like "Nashville" and "24".
Boothe was also nominated in two ensemble SAG Awards for "Nixon" (1996) and "Deadwood" (2007).
He is survived by his wife Pam Cole and two children children, Parisse and Preston.