Smith finished 22 of 29 with an interception for the Crimson (1-1). Devin Darrington ran for 91 yards and a touchdown and Aidan Borguet added 84 yards rushing and a score.
The Bears (1-1) scored 34 seconds into the game, capping a three-play, 75-yard drive with Allen Smith's 22-yard TD run.
Harvard tied it at 7 before the end of the first quarter on Smith's 12-yard pass to Cody Chrest.
Smith's 13-yard TD pass to Adam West make it 14-7 with 1:42 left in the first half. Brown went four-and-out to give Harvard a short field and Smith connected with Jack Cook for a touchdown with five seconds left in the half.
Smith threw his fourth TD pass to B.J. Watson on the Crimson's opening drive of the third quarter. Darrington and Borguet scored in the fourth quarter.
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