He was appointed by Pope Paul VI on 1 July 1974 and retired in 1996; he was succeeded by the Most Reverend George Pell (as he was styled at the time).

[2] The Royal Commission into Institutional Responses to Child Sexual Abuse found that Little had led a culture of secrecy in the Melbourne archdiocese designed to hide complaints against several priests and protect the church's reputation from scandal.

He was ordained by Cardinal Pietro Fumasoni Biondi, Prefect of the Sacred Congregation for the Propagation of the Faith, on 3 October 1950 in the chapel of the college.

During these years he was involved in pastoral work with the large number of migrants finding a new home in Australia, especially within the Italian community.

During his time as Archbishop of Melbourne his support of the education and renewal for the Catholic community expressed itself in such initiatives as the publication of the religious education guidelines, the launch of the RENEW program, the establishment of deaneries, and the "Tomorrow's Church" process.

[4] In the 1977 Silver Jubilee honours he was appointed a Knight Commander of the Order of the British Empire (KBE).

[4] In 2002 there were media reports that Little failed to address issues associated with the sexual abuse scandal in the Catholic archdiocese of Melbourne, specifically relating to Father Wilfred "Billy" Baker, of Gladstone Park, Eltham and North Richmond parishes.