From 1848 until the completion of Italian unity in 1870, his whole activity was devoted to the Risorgimento, as Garibaldian officer, political refugee, anti-Austrian conspirator and deputy to parliament.

In 1866, with the rank of colonel, he assisted Garibaldi in the campaign in the County of Tyrol, in 1867 fought at Mentana, and in 1870 conducted the negotiations with Bismarck, during which the German chancellor is alleged to have promised Italy possession of Rome and of her natural frontiers if the Democratic party could prevent an alliance between Victor Emmanuel and Napoleon.

General irritation was caused by his and Count Corti's policy of clean hands at the Berlin Congress, where Italy obtained nothing, while Austria-Hungary secured a European mandate to occupy Bosnia and Herzegovina.

In 1887 he received the knighthood of the Annunziata, the highest Italian decoration, and on 8 August 1889 died while a guest of King Umberto in the royal palace of Capodimonte near Naples.

[1] Cairoli was one of the most conspicuous representatives of that type of Italian public men who, having conspired and fought for a generation in the cause of national unity, were despite their valour little fitted for the responsible parliamentary and official positions they subsequently attained; and who by their ignorance of foreign affairs and of internal administration unwittingly impeded the political development of their country.