In a letter to Innocent XI dated April 29, 1687 he vowed to be a Catholic King and declared his readiness and willingness and that of his troops to obey any order of the Roman Pope.

In 1688, George headed an abortive coup against a Persian governor of the neighboring Georgian region of Kakheti, and attempted, though vainly, to gain Ottoman support against the Safavid overlordship.

In response, Shah Solayman deposed George and gave his crown to the rival Kakhetian prince Erekle I, who then embraced Islam and took the name Nazar-Ali Khan.

Abbas Qoli-Khan, the beglarbeg (governor general) of Ganja, was placed in charge of the government in Kakheti and commissioned to reinforce Erekle's positions in Kartli.

In 1696, he managed to stage a temporary comeback and helped his brother Archil to temporarily regain the crown of Imereti in western Georgia, but was eventually forced to withdraw from Kartli again.

He was granted the title of Gurgin Khan by the Shah and was appointed the viceroy of Kandahar province and sipah salar (commander-in-chief) of the Persian armies.

He subdued many of the local leaders and sent Mirwais Khan Hotak, a powerful chieftain of the Ghilji Afghans (Pashtuns), in chains to Isfahan.

A punitive expedition into the Afghan lands led by George's nephew, Kay Khusrau, ended in October 1711 disastrously with his death and the destruction of nearly his entire force of 30,000.