While interviewing Cooper for her 10 Most Fascinating People of 2015" special, the 86-year-old Walters reveals that she, like many, has a bit of a crush on the Oscar-nominated star.
"I could just sit and stare at you but that would take too much time," she tells Cooper in the interview. "But I, I find you very screwable."
Later in the interview, a flirtatious Walters asks if the Joy star, 40, knows he's handsome, adding, "I think you're handsome, I think you're sexy."
"Thank you," Cooper responds. "I think that I've grown to stop thinking about it. ... But sometimes I feel better than others. Yeah, I think it has a lot to do with feeling comfortable with yourself."
PEOPLE's Sexiest Man Alive 2011 continues, "And I know that I'm more comfortable with myself than I've ever been in my life, so maybe that makes me more attractive."
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Walters has been known to make candid remarks during and after many interviews with newsmakers over the decades.
In 1991, Walters also got jokingly flirty while interviewing the Teenage Mutant Ninja Turtles for her Oscars special. After Donatello kisses her hand, she calls him "Charming, you're everything I heard you were."
Fellow TMNT Michaelangelo followed that up with a compliment of his own, calling her a "dudette."
Barbara Walters Presents: The 10 Most Fascinating People of 2015 airs Thursday at 9:30 p.m. ET) on ABC.