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After attending primary school in his native town, Puiu studied at seminaries in Roman (1893-1896) and Iaşi (1896-1900), and later at the Bucharest Faculty of Theology, where he received a licentiate in 1905. On 22 December 1905, he became a monk at Roman, being ordained a deacon three days later. From January 1907 to July 1908, he studied at the Kyiv-Mohyla Academy. From 1905 to 1908, he was, as a deacon, attached to the Cathedral of the Holy Voievods, Roman, while in 1908 he was transferred to the Cathedral of Saint Nicholas, Galaţi. There, on 6 December 1908, he was ordained a priest, being elevated to the dignity of Archimandrite on 1 January 1909. Three months later, he was named director of the Galaţi Theological Seminary and Vicar of the Archbishopric of the Lower Danube. On 1 September 1918, he became director of the Chişinău Theological Seminary, being named Exarch of Bessarabia's monasteries two months later (soon after that province united with the Kingdom of Romania).
On 17 March 1921, Puiu was elected Bishop of Argeş. He was consecrated in that position on 25 March by Metropolitan of Wallachia Miron Cristea in the Bucharest Metropolitan Cathedral and invested into the office that day by King Ferdinand. Two days later he was installed in the episcopal chair at Curtea de Argeş Cathedral; he remained there for two years. In 1923 he became bishop of Hotin, where he remained until 1935. During his time in that position, he undertook a number of actions to try and improve the lives of the inhabitants of the Bălţi area, his seat being in that city. On 17 October of that year, he was elected Archbishop of Cernăuţi and Metropolitan of Bukovina, being seated on 10 November. In May 1940, he left that position and retired to a monastery (Puiu later claimed that this was due to a conflict with King Carol II due to the latter's alleged attempts to take Bukovina's riches for himself). While Metropolitan of Bukovina, Puiu had tens of churches changed from wooden construction to concrete, repaired a few hundred others, established eateries for foresters, and gave free wood to peasants (which helped rebuild the ski resort of Vatra Dornei).
Romania entered World War II in 1941, and Puiu served as Metropolitan of Transnistria at Odessa from 16 November 1942 to 14 December 1943. There, he reopened churches closed by the Soviet authorities, helped the needy, the poor and children, and helped educate people in the Orthodox faith. In August 1944, he was in Zagreb (present-day Croatia) for the ordination of an Orthodox bishop there, accompanied by a handful of Romanian priests. He sent the priests back to Romania, sure they would be safe, but decided to flee to the west, fearing punishment from the Soviets for his wartime religious activity in Transnistria. Indeed, a pro-Communist Romanian People's Tribunal sentenced him to death in absentia for war crimes on 21 February 1946.
For several years Puiu wandered around Europe, living for short periods in Vienna, Germany, Switzerland, Venice, Draguignan and Auvergne, before settling for good in Viels-Maisons, a village on the Marne River 96 km east of Paris. At one point during these travels, self-proclaimed Iron Guard leader Horia Sima offered Puiu the post of Minister of Religious Affairs in his government in exile, but the latter declined.
From 1948 to 1958 Puiu headed the Romanian Orthodox Church in France. Still a bishop, his church was subordinated to the ROCOR Metropolitan in New York City, and he used the Romanian Orthodox parish in Paris (established in the 19th century) as his cathedral. On 28 February 1950, the Holy Synod of the Romanian Orthodox Church in Bucharest, headed by Patriarch Justinian Marina and under pressure from the Communist authorities, deposed Puiu from his ecclesiastical position; he was rehabilitated on 25 September 1990. Among the reasons cited for this action was an allegedly pro-Catholic 1925 article he had written; for this, he was branded an "imperialist agent".
As of 1 April 1958, Puiu disbanded the Paris Archdiocese he had established a decade earlier. There were three main reasons for this action. First, its goal of uniting all Romanian Orthodox believers in Western Europe completely failed, as it never had more than one parish. Second, the church faced a constant clergy and financial shortfall. Third, its subordination to ROCOR isolated it within the wider Orthodox world. On top of all this, the church was riven by the political factionalism that marked the Romanian exile community. Thus, the church was returned to the priests who had led it before Puiu's arrival, and the bishop retired to Viels-Maisons, where he died six years later. He was buried in that village but later moved to Montparnasse Cemetery, where he lies today.
- Bishop of Argeş (elected 17 March 1921, consecrated 25 March, enthroned 27 March - served until 1923)
- Bishop of Hotin (seat at Bălţi) (elected 29 March 1923, enthroned 13 May - served until 1935)
- Metropolitan of Bukovina (elected 17 October 1935, enthroned 10 November - served until May 1940)
- Metropolitan of Transnistria (16 November 1942 - 14 December 1943)
- Bishop of the Romanian Orthodox Diocese of Western Europe (1948 - 1 April 1958)
- Dictionary of Romanian Theologians.
- (Romanian) Romanian Metropolitan Visarion Puiu, by Protohierarch Sorin Petcu, Müllheim, July 2006
- (Romanian) Visarion Puiu in the Dictionary of Romanian Theologians
- (Romanian) Statement regarding Puiu of 11 March 2003 in the Romanian Chamber of Deputies by Member of Parliament Pavel Târpescu