The Superbad star will play Dirty Randy in the third season premiere, the programme's executive producers announced at the Television Critics Association press tour.
Dirty Randy, who is a friend of Rafi (Jason Mantzoukas), has previously been mentioned on the show.
The League executive producer Jackie Schaffer said: "We made a promise to our fans last year that if FX brought us back for a third season, that they would meet Dirty Randy... We think it's going to be great."
Rogen, who previously starred on the TV show Freaks and Geeks, has worked on movies including Pineapple Express, Knocked Up and The Green Hornet.
Saturday Night Live star Will Forte has also signed up to appear in season three of The League and will play one of the "out-of-town guys".
"The guys are thrilled to see him," explained executive producer Jeff Schaffer. "But he's a little different than they remembered."
The League will return for its third season on October 6 on FX.
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