It goes back farther than that -- that game you referenced was in 1991, and he's been doing the chant since at least the 1980s.
From article with link posted above:
Big Red doesn't remember the exact year, either 1976 or 1977, but he knows it was a cold night at the old Greer Fieldhouse. The story of this incredible tradition goes something like this. Red and a friend were watching the Huskies struggling and the cheerleaders were not getting the crowd into it. As the squad does now, the cheerleaders spelled out the letters of UConn to the fans, but Red said the students weren't getting excited enough. That's when Big Red became a legend.
He stood up and yelled, "Are you ready?" and spelled out "UConn" with his arms while the crowd screamed, "U…C…O…N…N, UConn, UConn, UConn."