Wyly, who maintained a home in Woody Creek just outside Aspen, was turning onto a highway near the local airport when his Porsche was hit by a sport utility vehicle, the Colorado State Patrol said in a statement. Wyly was taken to Aspen Valley Hospital, where he died. The other driver suffered moderate injuries.
In Texas, Wyly and his younger brother, Sam, along with their wives, gave $20 million to help build Dallas' performing arts center. They also donated big, but quietly, to Republican causes.
"He is among the finest people I have ever known," William Brewer III, Wyly's attorney and long-time friend, said in a statement to The Associated Press. "His contributions in business, philanthropy and civic leadership will forever be remembered."
Wyly's family has donated almost $2.5 million to more than 200 Republican candidates and committees at the federal level over the past two decades, according to the nonpartisan Center for Responsive Politics. The brothers themselves had said they'd given about $10 million to Republican candidates and causes since the 1970s.
Texas Gov. Rick Perry was one of the biggest political beneficiaries, receiving more than $300,000 combined from the Wylys since 2000, according to Texas Ethics Commission reports.
Last summer, the Securities and Exchange Commission accused Wyly and his brother of using offshore havens to hide more than a half-billion dollars in profits over 13 years of insider stock trading. The brothers strongly denied the claims.
Charles Wyly was born during the Great Depression, and he was a child when the collapsed economy forced the surrender of his family's cotton farm in Lake Providence, La. Later, he and his younger brother starred on the high school football team, studied at Louisiana Tech University in the 1950s, and eventually set sales records at IBM.
They rose to the elite class of billionaires, A-list members of Dallas society and regular donors to philanthropic projects and primarily conservative Republican candidates and causes.
Leaders of the Dallas arts community were stunned by Sunday's news of Charles Wyly's death.
"Charles was a critically important force," Bill Lively told the Dallas Morning News, noting that Wyly played a key role in the development of a $354 million performing arts center, which has a theater named after the billionaire.
"He was always positive," said Lively, who launched the campaign to build the arts complex. "He was always optimistic."
Robyn Flatt, executive artistic director of the Dallas Children's Theater, said Wyly was a good friend who made "immeasurable" contributions to the Dallas arts scene.
"He was a true friend of the arts and our community, a friend who truly cared and who truly made a difference," Flatt told the Morning News.