Luis Fernando was born at Madrid, the younger son of Infante Infante Antonio, Duke of Galliera and of his wife, Infanta Eulalia of Spain. He was baptised with the names Luis Fernando María Zacarías; the name Zacarías is in honour of Saint Zechariah on whose feast day Luis Fernando was born. In 1899 Luis Fernando and his older brother Alfonso were sent to England to be educated by the Jesuits at Beaumont College. They remained there until 1904. Elisabeth de Gramont, Duchess of Clermont-Tonnerre, who chronicled various aspects of Parisian life in her four-volume memoirs, wrote about him: "The Infante was certainly the most divertingly cynical little creature who ever amused Paris. Slim, pallid, round- and restless-eyed like a bird, sullen looking, with lovely hands like those of a Coëllo Infanta, he promenaded his lubricous little royal person from drawing-room to awful bouges and then, ingratiatingly and affectionately, he would sink like an abandoned child at the feet of some 'Good Dame' and lament his lot."

On July 17, 1914, The New York Times reported the marriage of Luis Fernando to Beatrice Harrington. The newspaper was mistaken, however; the groom was actually Don Luis de Borbón, Duke of Ansola.

In October 1924 Luis Fernando was expelled from France. He was purportedly involved in the trade of illegal drugs. In response King Alfonso XIII of Spain deprived him of his privileges as an Infante of Spain.

Unable to reside either in Spain or France, Luis Fernando moved to Lisbon. In March 1926 he was arrested at the Portuguese-Spanish border disguised as a woman. Some smuggled goods were found in his possession, but no drugs. In 1927 he allegedly travelled to Italy in the company of Portuguese homosexual poet António Botto.

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