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It's a joke in the Glee fandom (mainly tumblr) that originated from Special Education, where Jeff (Riker) and Nick (Curt), tell Kurt that they've auditioned 3 and 6 times respectively (those were their only lines on the show). The fandom turned it into a running joke that they were Agents 3 and 6 of the "Three Six Mafia". The boys, being as involved in the twitter/tumblr fandom as they are, naturally found out about it and thought it was awesome.