Noted for his activities with the Filiki Eteria in the Danubian Principalities, he is considered to be a leading figure of the Greek Revolution.

Olympios became a supporter of the ideas diffused by Rigas Feraios for a common Balkan revolution against the Ottoman rule, and moved to Wallachia.

There, with the help of Constantine Ypsilantis, he composed a military force of Greeks to fight alongside the Russian Empire in the Russo-Turkish War of 1806.

Olympios married Čučuk Stana, the widow of Hajduk Veljko, who had arrived from Serbia to participate in the Greek War of Independence as a fighter, alongside his own men.

His widow and children fled to Khotyn, then part of the Bessarabia Governorate of the Russian Empire, where other people of the Serbian and Greek War, had taken refuge.