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son of George Plunkett, was born at Mount Plunkett, county Roscommon, Ireland, in June 1802. He entered Trinity College, Dublin, in November 1819, graduated B.A. in 1824 and in 1826 was called to the Irish bar. He practised as a barrister with success, fought for Catholic emancipation, and had much influence on the success of his party's candidates at the election for Roscommon held in 1830. In 1831 he was appointed solicitor-general of New South Wales where he arrived in June 1832. The then attorney-general, J. Kinchela, was so extremely deaf that it was difficult for him to do his work, and Plunkett had to undertake most of his duties. Early in 1836 Kinchela retired from his position, Plunkett took his place, and in the same year was associated with Governor Bourke (q.v.) in bringing about a new church and schools act. Plunkett obtained leave of absence to attend to private business in Ireland in 1841, and did not return to Sydney until August 1843. In October 1844 he applied for the vacant position of chief justice which was, however, given to Alfred Stephen (q.v.). Plunkett was offered the judgeship vacated by Stephen but declined it. He was made a member of the executive council in March 1847, and in 1848, when the national school system was founded, was appointed chairman of the board of education. He gave up the attorney-generalship and retired on a pension of £1200 a year in 1856. In the same year he was elected a member of the legislative assembly at the first election under the new constitution. He resigned his seat in January 1857, was nominated to the legislative council, and elected its president. In February 1858, on account of the board of education having issued regulations which Charles Cowper (q.v.), then premier, disapproved of, Plunkett was dismissed from his position as chairman and he thereupon resigned from the council. There was much public sympathy with Plunkett, and the government offered to reinstate him if he would withdraw statements he had made in letters which were considered offensive. This he declined to do. Plunkett was again a member of the legislative assembly from September 1858 to November 1860, in June 1861 was nominated to the council, and from October 1863 to February 1865 was vice-president of the executive council in the first Martin (q.v.) ministry. He was then reconciled with Cowper, and from August 1865 to January 1866 was attorney-general in the fourth Cowper ministry. He was also vice-chancellor of the university of Sydney from 1865 to 1867. For the last two years of his life he lived much at Melbourne on account of his wife's health, and he made his last public appearance there in 1869 as secretary to the provincial council of the Roman Catholic Church. He died at Melbourne on 9 May 1869 leaving a widow but no children. Plunkett was the author of The Australian Magistrate; a Guide to the Duties of a Justice of the Peace, first published in 1835 and reissued in at least three subsequent editions; The Magistrate's Pocket Book (1859), and On the Evidence of Accomplices (1863).

Plunkett was dignified and somewhat austere in manner, though he could relax on occasions. He had much ability and exercised great influence in the early days of education in New South Wales and in connexion with the anti-transportation movement. John Fairfax (q.v.) said he was "the greatest friend of civil and religious liberty in the colony", and he was in advance of his time in his attitude to the land question, and in his advocacy of manhood suffrage.