He was selected by Grand Prince Vasily III on July 27, 1511 and consecrated Metropolitan on August 3, 1511. He was said to be austere, never sycophantic to the grand prince, and never one to do anything against his own conscience. He was of the Non-possessors, those who opposed ecclesiastical land-ownership, although that group had been defeated at earlier church councils. He also protected Maximus the Greek, who was brought to Moscow to translate Greek texts.

In 1515, Varlaam consecrated the main church of the Khutyn Monastery just outside Novgorod the Great (the archiepiscopal see being vacant from 1509). That same year, he consecrated the Tikhvin Monastery, also in the Novgorodian Eparchy.

Due to a dispute with Vasily III, who wished to divorce his wife and remarry, a policy which the metropolitan opposed, Varlaam was removed from office on December 17, 1521. He was initially confined in shackles in the Kyrilo-Beloozersky Monastery north of Moscow, but was soon removed to the Spaso-Kamenyi Monastery in Vologda where he died sometime in 1522.

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