"Bibliothek" is a collection of books available for reading, and exceptionally also for borrowing. When you have a lot of books at home, you could call this your "Bibliothek".
"Bücherei" is also a collection of books, typically available for borrowing. "Leihbücherei" means lending library.
In an academic context, the university library is always called "Universitätsbibliothek", probably because the Greek word Bibliothek sounds more learned and posh than the German word Bücherei.