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It will not sync. The updated metadata for the books are stored in the file metadata.db. And if you copy the old library over the current you will end up with the old metadata and possibly a lot of unmaintained duplicate books.
Copy over the old library, but rename the folder first. Or rename the folder with text existing library.
After that you have two libraries. One old but functional and one new but corrupt. If you need to sync them you have to do that by manually copying books between the libraries using Calibre. Don't try to copy or change books inside the Calibre library manually any other way. There lurks chaos and corruption.
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