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OneDrive is not a good idea. It has a bad habit of randomly deleting books. I personally use Dropbox. The one rule that you always have to remember is to stop syncing while Calibre is open and never run Dropbox on both computers simultaneously, otherwise you'll get a messed up library in no time. Generally you should do things in that order:
1. Quit Dropbox or pause syncing
2. Open Calibre and do what's needed there
3. Close Calibre
4. Sync
5. When syncing is done, quit Dropbox
Now on the other computer:
1. Sync
2. Quit Dropbox or pause syncing
3. Open Calibre, do what's needed
4. Close Calibre
5. Sync
6. When syncing is done, quit Dropbox
Also you should run Library Maintenance regularly on both computers, because no matter how careful you are, errors still find their way in.
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