The museum resulted from the purchase by the city of the Buenos Aires home of Enrique Larreta, perhaps the most prominent Argentine exponent of Hispanic modernism in literature, and Ambassador to France from 1910 to 1919.

[1] The former Larreta home, designed by Argentine architect Ernesto Bunge,[3] for Francisco Chas Belgrano and his wife Catalina de los Remedios Salas and inaugurated in 1886, is a work of neo-Spanish colonial architecture, and features an Andalusian patio measuring 6,500 m² (70,000 ft²) and connected to the house via an extensive portico.

[4] Much as Martín Noël did with the property that later became the Isaac Fernández Blanco Museum, Larreta had the home expanded and refurbished along neo-colonial lines (restauración nacionalista, as the designs were known).

[5] The extensive gardens feature ginkgo biloba, ombú, wisteria, cypress, palm, bitter orange, and silk floss trees, as well as buxus hedges totaling around 700 m (2,300 ft).

The museum also includes the Alfonso El Sabio Library, specializing in Spanish literature, and La Casita de Arriba, a children's learning annex.