"I have a bit of a crush on Dax Shepard," Pitt said of Shepard, an actor known for Parenthood.
Shepard, who also hosts the Armchair Expert podcast, had voiced his crush on Pitt during a previous appearance on Ellen.
"He is an angel," Shepard said of Pitt. "This is someone that has fallen from the stars."
"The only thing that I love on par with sloths is Brad Pitt. Yeah, I have real strong, strong feelings about Brad Pitt. Always have," he said.
Pitt and host Ellen DeGeneres also discussed their shared dating history. Pitt and DeGeneres first met at a pool party hosted by singer Melissa Etheridge.
"I remember Melissa Etheridge's pool party, where I think you were hitting on my girlfriend," Pitt recalled. "I was flattered."
"I actually since then have dated another one of your girlfriends," DeGeneres said. "We'll talk about that later."
Pitt most recently starred in the Quentin Tarantino film Once Upon a Time in Hollywood. He will star in the new sci-fi movie Ad Astra, which opens in theaters Sept. 20. The film released a new trailer in August showing Pitt on a space mission.