You sound astounded that someone on the receiving side of legal action is trying not to cooperate. Next you'll be stating that him hiring a lawyer is proof of non-cooperation and evidence of guilt.
If you got to do overbroad things every time a defendant was "non-cooperative" it would apply to every single court case.
See my comment here[1]. While I'm not normally a government apologist, from the unsealed court documents, it appears that they did everything by the book here. The original order was for metadata related to a single, specific named account. There were several follow up orders and court proceedings before the request was broadened to turn over the SSL keys.
I'd claim that not producing evidence in response to a lawful subpoena and court order is proof that he's guilty of contempt of court[2].
[2] There are lawful ways to resist such an orders - you file a motion to oppose in the case. While I don't have access to PACER to confirm that no such motion was filed, the judge's orders have no mention of such a motion in the established facts.
dlgeek explains the entire situation better than I. However, I wanted to apologize for poor wording. It wasn't that he wasn't trying to cooperate. Rather, than it seemed like he was trying to be unreasonably uncooperative to what was a reasonable and lawful order (starting with the information/traffic of a single individual). The distinction is important, I think.
Considering that was far from the first thing they asked for, no. Were their goals reasonable? Yes. Was Levison trying to cooperate? No.