Her fourth Musart album, "La sentimental" (1964), includes both ranchera and bolero songs. It is her first album without mariachi arrangements; Benjamín "Chamín" Correa is credited as the album's guitarist. "La sentimental" peaked at number 9 on "Record World" Latin American LP Hit Parade. "Mi destino fue quererte" peaked at number 4 on "Record World" Latin American Single Hit Parade and became one of Flor Silvestre's signature songs. In December 1964, "Cashbox" ranked her among the top ten Mexican folk singers of the year. Her fifth Musart album, "La acariciante voz de Flor Silvestre", was released in 1965. One of the album's singles, "Una limosna", topped the "Record World" Latin American Single Hit Parade chart. The album also includes her hits "Gaviota traidora", "El mar y la esperanza", "Amor se escribe con llanto", and "Espumas". "Celosa con Flor Silvestre y otros éxitos" (1966), her sixth studio album for Musart Records, peaked at number 11 on "Record World" Latin American LP Hit Parade. The album's lead single, "Celosa", peaked at number 9 on "Cashbox" Mexico's Best Sellers and number 4 on "Record World" Latin American Single Hit Parade. "¿Por qué, Dios mío?", another single included in "Celosa", also charted well on "Record World" Latin American Single Hit Parade. In 1967, she released two albums, "Boleros rancheros con la acariciante voz de Flor Silvestre" and "Flor Silvestre, vol. 6", and made her last film of the decade, "El as de oros". In 1968, she released two albums, "Flor Silvestre, vol. 7" and "Flor Silvestre, vol. 8". "Flor Silvestre, vol 7" includes "Reconciliación", one of her major hits from the late 1960s, as well as several other hits, including "Cenizas de amor", "Cariño malo", "Triunfamos", and "Tres días". "Flor Silvestre, vol. 8" features arrangements by famous guitarist Antonio Bribiesca and composer Gustavo A. Santiago and includes the hits "No vuelvo a amar" and "Tú, sólo tú".