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It will break.
Calibre needs local files, not remote. It's using SQLight, not an SQL server, and if was running an SQL server you'd connect to that, not files, and there would still be a problem because the actual ebooks are not inside the database, though logically part of it.
One option is to run Calibre on the NAS (if it can) and start the Calibre Content Server.
You can't do what you have tried, and even what is working will break.
A second option is a "main" calibre on your PC with local files and rsync (grsync) to the NAS when Calibre is closed. Then on the other laptop(s), rsync from NAS (regarding it as read-only) to the laptop when Calibre closed. Only add ebooks, edit metadata or ebooks on the main PC. This is very reliable. Use rsync (grsync) to only copy newer files or delete files not on source. The grsync simply is a GUI to generate the rsync arguments.
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