In Game 2 of the American League Championship Series (ALCS) against the Baltimore Orioles, Cain added to his postseason highlight reel with yet another stunning, extra-base hit-stealing grab, this one of a J. J. Hardy line drive to right center field in the 6th inning to preserve a 4–4 tie. At the plate, he went 4-for-5, tying George Brett's franchise record for most hits in a postseason game, and drove in a 9th-inning run that helped seal the Royals' 6–4 victory over the Orioles, their sixth consecutive win in the 2014 postseason. Cain ultimately ended up winning the ALCS Most Valuable Player Award (MVP) award for his efforts at the plate as well as in the field. He finished with a .533 batting average, eight hits, five runs, and numerous spectacular defensive plays which helped the Royals to sweep the Orioles and move on to the World Series.