dougraid
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dougraid's post in Cache setup & sanity check was marked as the answerI'm pretty new to unraid myself so take this with a grain of salt. I think the answer depends on your objective, what you hope to gain. I appears you have good VM performance since they are on your current nvme drive. Is space the issue? If that is the case, then upgrading would keep your speed while improving your available storage. If redundancy is important, then I think that answers your question. 2 x 2TB NVme drives in Raid 1 would be nice for sure.
I've heard good things about Segate Firecuda NVme drives for durability and performance. The 2TB versions were on Amazon for $129 each not too long ago (maybe they still are).