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Calibre is not a multi user program! But yes, it is possible, in a fashion. Just use copies of the library stored on the NAS. So strictly speaking the computers can freely access copies of the same library simultaneously.
There are a lot of sync tools you can use to very quickly update a local copy on a PC from the master library on the NAS. The only limitation with this is that it is becomes difficult to manage updates to the library. Changes may overwrite each other, and corrupt the library, if you sync changes back to the NAS from more than one computer. If you only allow updates from one computer, then it is no problem.
You can automate the sync process by adding some commands to the script that is used to start calibre, or by manually running the sync when needed.
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