Carlos was born at the Royal Palace in Madrid on 31 January 1818, the elder son of Infante Don Carlos Maria Isidro. On 10 July 1850, he married Maria Carolina of the Two Sicilies, fifth daughter of Francis I of the Two Sicilies. They had no children.

In 1860, during a Carlist rising, he and his brother Infante Don Fernando were taken prisoners at San Carlos de la Rápita. Although they were later released, in 1861, suddenly and unexpected, Carlos Luis, his wife Maria Carolina, and his brother Fernando died, for reasons not fully explained. The three are buried at Trieste, in the chapel of Saint Charles Borromeo in the Basilica di San Giusto. Don Carlos Luis was succeeded as Carlist claimant by another brother, Juan, Count of Montizón.