Antony Cardinal Padiyara was nominated the first Bishop of the new diocese. He was a great visionary who directed the destinies of the diocese for 15 years. He established 17 new parishes, built 28 new churches and chapels and invited new religious congregations to help in the work of consolidation and extension. He remains the Architect of the diocese of Ootacamund who succeeded in laying solid foundations for the future. On 13th June, 1970 he was appointed Archbishop of Changanacherry in Kerala. He left the diocese of Ootacamund on 14th August, 1970 and later he became a Cardinal.

The next Bishop was Archbishop Packiam Arokiaswamy from the neighbouring diocese of Coimbatore. He was nominated on 6th February, 1971, and was ordained Bishop on 28th April, 1971. His tenure was very short and within a brief span of hardly ten months, he was promoted as Archbishop of Bangalore on 10th February, 1972.

On 21st December, 1973, the announcement of the nomination of Archbishop Aruldas James, who was at that time Rector of St Peter's Seminary, Bangalore as the Bishop of Ootacamund was a moment of joy and jubilation. He took charge of the diocese on 13th February, 1974 and was consecrated as the Bishop of Ootacamund on 20th February, 1974. New life and enthusiasm were generated after the arrival of Bishop Aruldas James. His hard work and strenuous efforts saw the diocese making tremendous progress in all levels as far as the spiritual, social, educational and developmental affairs in the diocese are concerned. He took special interest and practical concern in the spiritual and material wellbeing of the souls entrusted to his care. After leading the diocese for more than 20 years, like his predecessors he too was promoted as the Archbishop of Madras-Mylapore on 14th May, 1994.

It took more than two and a half years to hear the good news of the appointment of Archbishop Antony Anandarayar as the Bishop of Ootacamund on 12th January, 1997. His Eminence Cardinal Simon Lourdusamy consecrated him on 29th January, 1997 amidst great pomp and rejoicing manifested by the large attendance of bishops, priests, religious and people from all walks of life. His devotedness and kindness made him the good shepherd. Magnificent churches, beautiful chapels in substations, and presbyteries had been constructed. Archbishop Antony Anandarayar had created a new parish and had been responsible for inviting new religious congregations in the diocese to labour for the poor and oppressed in Chimitahalli, a remote parish in the diocese. He was also striving to make parishes self-sufficient and had introduced the slab system wherein parishes according to their income had the obligation to contribute a certain percentage to the diocese annually. The diocese was divided into five vicariates, each with a Vicar Forane for better co-ordination and administration. His love for the poor and downtrodden was exhibited by visiting the families in the slums. His primary concern had been providing education to the poor children that they might have a better future. In this venture he had upgraded St Francis Xavier's High School, Peria Kodivery to a Higher Secondary School. Thousands of poor children looked up to him as a loving father for the help he had offered for their betterment and improvement. He educated many children at various levels in schools and colleges. His motto “to serve in faith and love” had become an attainable reality by his extension of maximum help to the poor and downtrodden. In 2004 he was appointed as Archbishop of Pondicherry-Cuddalore.