Davon Marshall drained six 3-pointers en route to 20 points as the Flames (15-20) won the Big South Tournament title game, capturing their first league crown since 2004.
Tavares Speaks also played a big role in the win, providing 18 points, nine rebounds, four assists and two steals.
The victory earned Liberty -- which began the season with eight straight losses -- an automatic spot in the NCAA event.
They tied the 2008 Coppin State squad for the most losses entering the national tourney.
The top-seeded Buccaneers (19-12) were paced by Saah Nimley with 18 points.