The app downloads to your device what I'd call a catalogue of all contents in the library you point it too.
In my case I point it to a calibre-web database. Calibre-sync then downloads all book titles / metadata (including series data) and book covers. I believe the downloading of covers is optional.
I'm then able to browse the library on my phone and download any actual books I want.
Calibre-sync does not in itself copy data from your calibre library to any of the locations it supports such as OneDrive or Google Drive; rather it depends on YOU having a process to copy data to the location in question.
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