Born on December 1, 1878, in Surrey, England. His mother died at childbirth, and the youngest child of the Reverend John Kay, a Congregational Minister. George was adopted by his aunt, Francesca Arundale, a dear friend of Madame H. P. Blavatsky whom she invited to her home in London. She joined the Theosophical Society in 1881, and George joined in 1895. HPB and Colonel Olcott had great affection for George. When George was seventeen, he was admitted to the London Lodge by A. P. Sinnett.

George was an English Theosophist, editor, writer, educator, and Occultist. In 1900 he was graduated from St. John’s College, Cambridge, and Joined International Co-Freemasonry in 1902. Went to India at Dr. Besant’s request in 1903 as Professor of History at the Central Hindu College, Benares. 1913-1915 established movements to help J. Krishnamurti and his brother Nityananda to help them in their education and work. By 1916 returned to India joining Dr. Besant as Organizing Secretary, All-India Home Rule League. 1917 George founded at Madras under the Theosophical label for Promotion of National Education, for which he established schools and education everywhere in India, his chief activity at the national University, Madras, of which Rabindranath Tagore was chancellor. In 1920 became Minister of Education in Indore, India. Married Rukmini Devi, daughter of Pandit Neelakanta Sasrti, Madras 1920. In 1925 travelled extensively in Europe and America, becoming Regionary Bishop of the Liberal Catholic Church in India 1926, visiting both countries every year from 1931 to 1934. Also in 1926, he became General Secretary in Australia with Bryon Casselberry serving as Assistant General Secretary.

He became President of the Theosophical Society June 1934, elected for seven years in Succession to Dr. Annie Besant. By 1935 he became Most puissant Grand Commander Eastern Federation, British Empire, and Representative of Supreme Council. Dr. Arundale was presented with the Subba Row Medal for his contributions to Theosophical literature in 1935. George gave lectures on Symbolic Yoga in 1937 appearing as a book "The Lotus Fire": A Study in Symbolic Yoga. By 1945 became gravely ill and passed away on August 12, 1945.