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Historically: The Cleveland Browns have the highest historical winning percentage during the Superbowl era of any team never to actually win a Superbowl. In addition, the Cleveland Browns were generally regarded as one of the best teams outside of the old NFL in the pre-Superbowl era, playing in the now defunct AAFC.
In any one season: The best team to "not" win a Superbowl would probably be the New England Patriots of 2007, who were the only team to 16-0 and were upset in Superbowl XLII by a couple of freak plays (as well as an impressive effort from the Giants).
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