Claimant to the Spanish and French thrones
On 18 July 1909 Jaime succeeded his father as Carlist pretender to the throne of Spain and likewise inherited the Legitimist claim to the throne of France. As Carlist pretender to Spain he was known as Jaime III, but used the style Duke of Madrid. As holder Legitimist claim to France by so-called Blancs d'Espagne he was considered to be Jacques I, but often referred to as Duke of Anjou.
Jaime retired from the Russian army and henceforward lived mostly at Schloss Frohsdorf in Lanzenkirchen in Austria and at his apartment on Avenue Hoche in Paris. He visited Spain incognito on a number of occasions. He also owned the Villa dei Borbone at Tenuta Reale near Viareggio in Italy which he had inherited from his mother.
For part of World War I Jaime lived under house-arrest at Schloss Frohsdorf in Austria.
On 16 April 1923, by a decree to his Delegate-General in Spain, the Marques de Villores, Jaime created the Order of Prohibited Legitimacy (Orden de la Legitimidad Proscrita) to honour those who suffered imprisonment in Spain or were exiled for their loyalty to the Carlist cause.
In April 1931 the constitutional king of Spain Alfonso XIII was forced to leave the country and the Second Spanish Republic was proclaimed. Jaime issued a manifesto calling upon all monarchists to rally to the legitimist cause. Several months later, on 23 September, Jaime received Alfonso at his apartment in Paris. Two days later Alfonso and his wife Ena received Jaime at the Hotel Savoy d'Avon near Fontainebleau. Jaime conferred the collar of the Order of the Holy Spirit upon Alfonso. These meetings marked a certain rapprochement between the two claimants to the Spanish throne. According to some authors – contested by the others – the two signed or verbally agreed an arrangement named Pact of Territet which would terminate the Alfonsist-Carlist discord.
A week after his meetings with Alfonso, Jaime died in Paris. He was buried at the Villa dei Borbone at Tenuta Reale. He was succeeded in his Spanish and French claims by his uncle Alfonso Carlos, Duke of Anjou and San Jaime.