Ryan Kemrite added 17 points and Georgie Pacheco-Ortiz had 10 points for the Flames (2-0), who defeated an ACC opponent for the first time in nine years.
Wake Forest dropped to 0-2 for the first time since the 1979-80 season.
Bryant Crawford's 21 points paced Wake Forest, with 17 coming in the second half. Keyshawn Woods and Doral Moore each added 14 points for the Demon Deacons, who shot 2-for-17 on 3-pointers.
Liberty made 9 of 21 shots from long range.
The Flames grabbed a 12-point lead in the opening minutes of the second half before Wake Forest scored nine points in a row.
Liberty responded for a 53-43 edge on freshman Keegan McDowell's 3-pointer. The score stood at 59-47 with less than 6 1/2 minutes to play.
Another McDowell 3 stretched the lead to 66-56.
Liberty, which hadn't won a Division I non-conference road game since Dec. 31, 2012, at Western Carolina, held a 39-28 rebounding edge.
Scottie James, who scored nine points, pulled in 14 rebounds for the Flames.
The Demon Deacons went the final 3:25 of the first half without a field goal then went almost another minute in the second half before Moore's short jump.
Wake Forest was 1-for-9 on first-half 3-point attempts.
Moore scored eight of Wake Forest's first 15 points.