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The Library was commissioned when the Monastery was headed by the Abbot Frei Bento de Siqueira around 1640. It housed books bequeathed by the Infante Luís (son of Manuel I), other books donated to the monastic community, some by monks who died, as well as books that were bought. When the monastery was closed, the library held around 8,000 volumes. The bookshelves, which were of maple wood, disappeared. Most of the books were lost, except for a batch that went to the National Library (printed works), the Torre de Tombo archives (manuscripts) and to the Casa Pia in Lisbon.

Exhibition: Today the Library space houses a permanent bilingual exhibition entitled "A Place in Time", the aim of which is to build a memory of the Monastery over 500 years, linking its history, and that of the Tower of Belém and the surrounding area, with the history of Portugal and the world.