Descendant of a Souliot family. He enrolled at the Law School in 1894 but the following year he entered the Military School of Evelpidon from which he graduated as an Infantry Lieutenant in 1900. He served in the Army Cartographic Service and taught Geography at the Evelides School. He took an active part in the Macedonian struggle, founding the secret Organization of Thessaloniki and collaborated with Consul L. Koromilas.

In 1908 he founded with Ion Dragoumis the secret Organization of Constantinople, which worked for the equal cooperation of the peoples of the Ottoman Empire, serving the Great Eastern Idea. It collaborated with the Liberal Party of Prince Shebahedin for the succession of the Sultan and the democratic governance of Turkey.

As a reservist he took part in the Balkan wars, serving as a liaison officer at the Bulgarian General Headquarters. Souliotis alerted King Constantine in time to the hasty movements of the Bulgarian army for the capture of Thessaloniki. Thus the Greeks managed to capture it first. He then served in various diplomatic missions.

In 1915 he became the Prefect of Ioannina and then the Prefect of Constantinople. In 1918-19 he was deported as a royal in Crete. In 1920 he was elected as a plenipotentiary of Thessaloniki in the Third National Assembly. In the same year he was promoted to Lieutenant Colonel. In 1922 he was demobilized. In 1934 he was Prefect of Florina and in 1935 he was appointed General Prefect of Florina. In 1934, he was appointed in 1934 as Governor of Thrace.

The life of Athanasios Souliotis was a great historical novel. With I. Dragoumis and G. He reissued the Political Review. He wrote political-historical works, The Macedonian Struggle, The Organization of Thessaloniki, The Organization of Constantinople, Memoirs, Note etc.