Singular? Only one?! Most important? First?
I'd have to go with the defensive finale of the 1971 (1970 season) Orange Bowl. In particular Willie Harper's strip of Bert Jones, which unfortunately did not ice the game. It was Terrio's interception of Jones that finally put the game away. Tagge's TD came with 8:05 left. We let Jones convert a 3rd and 29 from their seven. Then came Harper's play. Unfortunately, Tagge fumbled the ball away (on a third and long run) and Terrio picked off Jones. Little did I realize how good a QB Bert Jones was (NFL career felled by a bad shoulder). [Edit: Harper had a monstrous game; after Tagge’s TD he blocked/ forced a four yard punt, which we should have iced the game but fumbled it away deep in LSU territory. Early in the game he recovered a fumble. He was named outstanding lineman. ]
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Basically, that game was finally everything falling into final place after things started falling our way with the ND defeat of USC and us beating OU in November. All of the other New Years games going our way.
My earliest memory was probably Dennis Claridge's TD run in the Orange Bowl against Auburn. Then three straight bowl losses with the NC on the line in the first two (Arkansas in Cotton Bowl, 'Bama the next year in the Orange Bowl). Then Kenny Stabler and Ray Perkins hammering us in the next Sugar Bowl... (throw in a loss or two against OU) and then the miserable 6-4 years, which was when I started attending games in Lincoln.
Big things started in 1969 with Van Brownson and Jerry Tagge taking over the QB duties, we wiped out OU in Norman in 1969 with clobbering Georgia in the Sun Bowl. That set up our rising run in 1970 season and the OB above put everything in place that a sixth grader could dream of. Then the next year was even more spectacular.