You certainly can do that if you have enough slots on your motherboard. You need to make sure you have two M.2 Slots on the motherboard. Many motherboards like this
Gigabyte Z370 Board have an M.2 Slot and an additional "Optane Ready" slot.
The caveat here is that you may not see the performance boost you are looking for. At 64 GB, the Optane module you mentioned will only be able to cache at most 64 gigabytes of data, the equivalent of 1 - 5 games. My understanding is that Optane only caches the most used data (as determined by a proprietary software algorithm). I was initially looking into a set up like this, but thought the performance gains on 64 - 100gb of data was not worth the price of the Optane module.
Would love to hear other opinions from the community. It's still difficult to ascertain the raw performance increase resulting from Optane caching.