In 2007, Natalia had a participation (featuring) in the album "Real" of the Puerto Rican singer Ednita Nazario, performed a duet song "No", (composed by Armando Avila and self Natalia). This song only appears on the album Ednita Nazario.
"The Best Thing About Me Is You" is Ricky Martin's new single with the original English version of the song features singer Joss Stone, while its Spanish version, "Lo Mejor De Mi Vida Eres Tú", replaces Stone's vocals with Natalia Jiménez.ref>quemovida.excite.es</ref>
On November 12, 2010, after appearing and performing at the 2010 Latin Grammys with Ricky Martin, Natalia announced her solo album and said she hopes to release her first single in January. She also announced that the band, La Quinta Estacion was not broken up and that her and Angel Reyero, her bandmate, were focusing on solo projects. She said "The band is still there, everything is still there, one day we will release another album [as La Quinta Estacion]"..
Natalia's first single as a solo artist "Por Ser Tu Mujer" was released on April 5, 2011. Her self-titled debut album "Natalia Jimenez" was released on June 21, 2011 in the United States.