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  • Steve Carell as Felonious Gru,former villain turned father.
  • Kristen Wiig as Lucy Wilde, an Anti-Villain League agent and Gru's love interest/new partner. Wiig also played Miss Hattie in the first film.
  • Benjamin Bratt as Eduardo Perez/El Macho, the owner of Salsa & Salsa, a Mexican restaurant in the Paradise Mall. Al Pacino was originally cast in the role, but left the film due to creative differences.
  • Miranda Cosgrove as Margo, the oldest of the three girls and the most overprotective of the trio.
  • Elsie Fisher as Agnes, the youngest child of the three girls, who is obsessed with unicorns
  • Dana Gaier as Edith, the middle and tomboy of the three girls
  • Russell Brand as Dr. Nefario, Gru's elderly, hearing impaired gadget man
  • Ken Jeong as Floyd Eagle-san, an owner of a wig store. Jeong also voiced Talk Show Host in the first film.
  • Steve Coogan as Silas Ramsbottom, the head of the Anti-Villain League
  • Moisés Arias as Antonio Perez, Margo's love interest and Eduardo's son
  • Nasim Pedrad as Jillian, Gru's irritating matchmaking neighbor
  • Kristen Schaal as Shannon, Jillian's superficial friend
  • Pierre Coffin as Kevin the Minion, Bob the Minion, Stuart the Minion, Additional Minions, and Evil Minions. According to Coffin, he lent his voice to 899 Minions.
  • Chris Renaud as Additional Minions, Evil Minions, and Italian waiter
  • Vanessa Bayer as Flight Attendant