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A staunch supporter of Greek Prime Minister Eleftherios Venizelos, his fortunes were linked with those of the Venizelists. The expulsion of King Constantine in 1917 allowed Meletius' installation as Archbishop of Athens, but the 1920 electoral defeat of Venizelos allowed the king's return and Meletius' [[deposition]]. His replacement as Archbishop was the Royalist Archbishop [[Theoklitos I of Athens|Theocletos]], the man whom he had displaced two years previously.
During his tenure as Archbishop, he tried to apply order to the patchwork of independent "trustee" Greek [[parish]]es in America by applying a 1908 Patriarchal decree that gave episcopal oversight of the Americas to the [[Church of Greece]], and even visited America in the summer of 1918 to survey the situation. Upon his return to Greece three months later, he appointed Bishop [[Alexander (Demoglou) of Rodostolou|Alexander of Rodostolou]] as his resident American legate. Alexander was delegated the unenviable task of initiating canonical order among the independent Greek parishes throughout North America.
While Archbishop he also journeyed to England where he conducted talks concerning the union between the [[Anglican Communion|Anglicans]] and the Orthodox Church.
