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Keeping your active Calibre library in OneDrive is not recommended. Best to keep a backup copy there. For that purpose many of us use FreeFileSync, the mirror sync option (certainly not two-way sync!). It will mirror any changes from your active library to the backup library, so you don't have to copy the whole library over every time you make changes.
Yes, you can install your library and settings on a new computer. There is an export-import option for that, but personally I have just copied the library folder and the settings folder over in their entirety and pointed the new Calibre installation to the library folder (right-click on the Library icon, Create/Switch, Use existing).
The settings folder is usually located (on Windows) in User/AppData/Roaming. You have to copy over the whole folder named calibre, to the same location on your new computer.
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