Humor. Skill. Wit. Sex appeal. That order.

life:

He had the requisite looks, charm, and talent — but it wasn’t until 1969 that Robert Redford truly broke out, guns blazing, as a Hollywood stud.

That was the year of Butch Cassidy and the Sundance Kid, and also the year that LIFE photographer John Dominis spent a week with the mustached man’s man, as the star mixed business and pleasure at his homes in Utah and New York.

Only a few of the photos Dominis captured made it into the February 1970 LIFE cover story. Here, LIFE presents an entire series of marvelous, unpublished photos of the Hollywood stud.