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The origin of the Archive of the Liberator can be dated back to 1813, when Simón Bolívar (1783-1830), still in his Brigadier days, began to copy and classify the correspondence he received, along with drafts of letters sent. The first custodian of this invaluable collection of testimonies about the past was the Liberator himself: Bolívar travelled with his archive. After his death, aides and close associates set about the task of continuing to collect Bolívar's documents. Among them, Daniel Florencio O'Leary and Juan de Francisco Martín were the most industrious in the methodical work, not only of keeping and conserving the documents treasured by the Liberator, but also of obtaining and collecting many other documents in the hands of contemporaries, including some of Bolívar's enemies. For almost two centuries the Venezuelan State has persisted in the work begun by Bolívar and his collaborators, which it continues to this day.

The archive includes political and military documents, personal letters, trials, proclamations, decrees, family documents, and other documents of various kinds. This documentation is a direct testimony of the life and deeds of the Liberator and of part of the history of the republics he liberated, as well as being an exceptional source for the study of the social history and ideas of 19th-century Latin America.

The Simon Bolívar Archive was inscribed on the Memory of the World International Register in 1997 and on the Regional Register for Latin America and the Caribbean in 2011.