I'm sure Larry was involved in Student Council in some way (the script on IMSDB.com says he's the outgoing president), so he wanted to make sure the vote counting was fair and impartial. And I think he was insulted that Jim kept insinuating that he made a mistake in counting, when it was clear he didn't.
Related question: when Jim reports to Walt's office the next day and finds Walt holding the two discarded ballots, both Larry and the janitor are there. I've always wondered if Larry went to the janitor and specifically asked him to check Jim's garbage can for the ballots when he emptied it? Or if the janitor found the ballots himself and reported it to Walt (because of the Chinese food incident at the beginning of the movie), and they called Larry to the office too because they wanted him to know they believed he counted correctly?
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