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The actor - who is married off-screen to actress Catherine Keener - has been starring in a three-episode stint on Friends as Aniston's office rival and latest love interest.
The gig on television's most popular comedy comes just as Mulroney is enjoying the critical and commercial success of Schmidt, in which he stars opposite Jack Nicholson.
While both roles are in comedies, Mulroney says the two experiences couldn't have been more different.
"I had never been on a sitcom. I have friends who are writers on shows, so I know how it goes, but when you're there it's like being in the trenches, you know. It's fast. It was actually quite the opposite of About Schmidt," the actor tells The Sun.
"The point of Friends is to be funny. If a line that was written to get a laugh doesn't get a laugh in front of the audience, they write another line and you shoot it again. It takes your breath away. The writers are just amazing. They produce a hilarious show every week."
Helping was that Mulroney knew many of the cast members going in. He went to college with David Schwimmer and has been friends for years with both Aniston and Courteney Cox.
"It was a perfectly natural gig to do," he says. "It was great working with Jen - she's just hilarious."
That said, being Aniston's new boyfriend has its advantages - namely the love scenes.
"It's a little bizarre kissing your buddy," he laughs. "But, you know, a lot of friends have made out with other friends."
The question of whether he may return in future episodes is up to the writers, he says.
"I'd be happy to, sure. But there aren't that many actors who get to have guest spots over multiple episodes, so to even get three is great."
In Schmidt, Mulroney plays Randall, the dubiously coiffed Midwestern waterbed salesman who is about to marry the daughter of Nicholson's Warren Schmidt.
What elevates the film to both the critical smash and Oscar contender it has become is, unlike many Hollywood comedies that would take the low road, About Schmidt treats its offbeat characters respectfully.
Randall, despite all his obvious shortcomings, never quite turns into the buffoon audiences might expect.
"I love Randall and I respect him. I knew from the start when we were creating his look that we did not want to make fun of him because we'd be doing what Warren Schmidt is doing and Schmidt is actually wrong about Randall," Mulroney says.
Grounding the movie during filming was Nicholson, who brought none of his devil-may-care persona to the set.
"Nicholson was very serious approaching his role. He was all business. He didn't dine out at the restaurants with the rest of us. He kept to himself. But it was a beautiful thing to see him work," he says.
An actor in Hollywood for more than 17 years, Mulroney's credits include such diverse films as Copycat, Young Guns and My Best Friend's Wedding.
That elasticity helped Mulroney land the unlikely role of Randall, but it also means that blockbusters don't come his way often, if ever.
"I don't have much say in the parts I get," he says candidly.
"I have more say in the parts I decide not to pursue. I'm really more interested in pursuing material like Randall, than something just to be in the mainstream. But I'm also not offered Jerry Bruckheimer films. Those don't come to me."
Which is no problem for the actor who has managed to dodge unemployment without ever getting caught up in what he calls Hollywood's "machine," in which young actors pop up as the Next Big Thing on magazine covers and then just as promptly vanish.
"When I show up on a magazine cover, the bell may toll," he laughs.
"I haven't tried to put myself forward. I don't think young actors do, but they get plugged into the machine and that's something I've always avoided ...
"I don't know why I've had the run I've had. I just keep my fingers crossed and try to make smart decisions that are creatively rewarding.
"I know it sounds corny, but it does actually mean something."
And there is at least one advantage to ducking bad films, he notes.
"You have to talk people into thinking it's a good movie and that's really no fun."