In 1827 he moved to Madrid, where he debuted on 14 September at the Teatro de La Cruz singing Otello by Rossini.
He moved permanently to Madrid in 1837, where he was a professor and served as a conductor and an occasional composer.
In 1839, he made his Spanish opera debut at the Teatro de La Cruz.
The latter was leader of the Teatro de la Cruz in 1840–1846, and for his company Basilio composed several operas including El contrabandista, El ventorrillo de Crespo, La pendencia, El diablo predicador (claimed to be his greatest success, with text by Ventura de la Vega [es], 1846).
Basilio Basili was one of those who attempted to revive the tradition of Spanish musical theatre.