On October 12, 1548, Diego Ruiz de Vallejo left El Tocuyo, under orders of Juan Villegas, to conquer the Cuicas Province, a name that was given by the natives that inhabited the area and where the Boconó valley was located, with the objective of taking gold from the mines that were supposedly in the area.

The Spanish Empire reacted by imprisoning and exiling Don Miguel Uzcátegui, Mayor of the city.

On two occasions (June 26–29, 1813 and March 10, 1821), Simón Bolívar visited Boconó, where he installed a base at Boca del Monte.

While in Boconó, he stayed at the house of Mayor Jose María Baptista, expressed his admiration of the region, and declared the city "Garden of Venezuela".

The municipality was originally divided into 13 parishes (Ayacucho, Boconó, Burbusay, Campo Elías, El Carmen, General Ribas, Guaramacal, Monseñor Jáuregui, Mosquey, Rafael Rangel, San José, San Miguel, and Vega de Guaramacal); Campo Elías separated to form its own municipality on January 30, 1995.