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I have to go with Wisconsin beating Nebraska in the 2012 Big Ten Championship Game.
But the most improbable upset I've seen in college football was Auburn shocking Alabama on Chris Davis' 109 yards missed field goal for a touchdown in the 2013 Iron Bowl. This was the season after when the Crimson Tide beat Notre Dame in the BCS National Championship Game.
As a NC State fan, there are lots of memorable games that include last second wins at UNC on a season long field goal, the complete domination of Notre Dame in the Gator Bowl, etc. That said, I think that the 1986 match-up with South Carolina is my most memorable. Seemingly out of reach, the Wolfpack won the game after a defensive lineman for USC went offsides on the final offensive play for NC State as the clock ran out. Since a game cannot end on a defensive penalty, the Wolfpack was given one last play from scrimmage with 0 on the clock. The play resulted in a TD as the desperation Hail Mary pass is completed to Danny Peebles in the end zone. NC State and South Carolina had a long standing rivalry that was pretty much a knotted affair in the W/L column over time. Unfortunately that rivalry "ended" when USC joined the SEC.
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