The Natalia Aróstegui Bolognini Collection contains poems, articles, extracts and off-prints, and music scores by important early/mid 20th century Cuban composers. Music scores include autographed manuscript music scores by Gonzalo Roig, an important Cuban musician of the mid-twentieth century; autographed music scores by Ernesto Lecuona, one of the most important and internationally known Cuban musicians of the 20th century; and sheet music by Jorge Anckermann, Eusebio Delfín, Gisela Hernández González, José Marin Varona, Jorge Mauri, and Ernestina Lecuona, Ernesto Lecuona's sister.

This collection also contains manuscript poems by Dulce María Loynaz del Castillo, a renowned Cuban poet and the 1992 recipient of the Cervantes Award of Literature; and documentation about Dr. Gonzalo E. Aróstegui y del Castillo, Aróstegui's father.