Upon graduation, Valladares taught briefly before moving to Paris in the early 1950s and forming a music duo with María Elena Walsh.

From the early 1970s, Valladares built bridges with popular musicians, playing other styles, like rock, in an effort to stop the commercialization of music.

When the Argentine dictatorship ended in 1983, she joined the Movement for the Reconstruction and Development of National Culture and worked with other musicians to present and preserve the country's musical heritage.

[3] As teenagers, they formed a group called Fijos (Folkloric, Intuitive, Jazz, Original, and Surreal) made up of Adolfo Abalos, Manuel Gómez Carrillo, Gustavo "Cuchi" Leguizamón, Enrique "Mono" Villegas, Rodrigo Montero, and Lucía Claudia Bolognini Míguez, later known as Lois Blue.

She was also interested in avant-garde poetry[3] and studied German philosophers, including Franz Brentano, Immanuel Kant, and Oswald Spengler.

[7] Valladares began publishing poems in regional magazines such as El mar (The Sea) in 1940 and the following year in La pirámide (The Pyramid).

[9][Notes 1] In 1941, while attending Carnival festivities in Cafayate, she first encountered Baguala [es], the folkloric style of music from the Province of Salta.

[12] On successfully completing her studies in philosophy and education in 1948, Valladares traveled to Europe with her mother and a friend, Nelly García Alvarez.

Upon her return to Tucumán, Valladares read Otoño Imperdonable (Unforgivable Autumn), a book of poems, and began a correspondence with the author, María Elena Walsh.

[15][16] During the two months they spent aboard the ship, Valladares taught Walsh, who did not have a musical background, the folk songs and rhythms she knew.

[14][15] Arriving in Paris, Valladares and Walsh established a gathering place in their apartment and put together a repertoire which included various folk music styles from Argentina.

Though American ethnomusicologist, Alan Lomax, acknowledged the quality of their music, he refused to produce it, because as members of the upper classes, their songs were not authentic.

[22][Notes 3] In 1966, Jorge Prelorán, a documentary filmmaker, approached her to advise both him and folklorist Augusto Raúl Cortazar on the musical portion of their film Relevamiento cinematográfico de expresiones folklóricas argentinas (Cinematographic Survey of Argentine Folkloric Expressions).

Their collaboration led to a series of short films, including Hermógenes Cayo and Valle Fértil (Fertile Valley) produced jointly with the National University of Tucumán.

Dressed in a poncho, she became a symbol of a countercultural movement against the commercialization of music that moved it away from its spiritual roots, bringing her into contact with both rock and classical musicians.

[31] With the end of the regime and a return to democratic rule in the early 1980s, Valladares joined other musicians in the Movement for the Reconstruction and Development of National Culture.

[35] For her work in mapping Argentina's musical heritage, Valladares was honored as the inaugural recipient of the National Prize for Ethnology and Folklore in 1996.