Athlumney was returned to Parliament for Drogheda in 1837, a seat he held until 1852, and served under Lord John Russell as Under-Secretary of State for the Home Department from 1846 to 1847 and as Chief Secretary for Ireland from 1847 to 1852 during the worst of the Great Famine.
He lost his seat in the 1852 general election, but was successfully returned for Canterbury in 1854, and continued to represent this constituency until 1865.
In 1863 he was raised to the Peerage of Ireland as Baron Athlumney, of Somerville and Dollarstown in the County of Meath, and in 1866 he was further honoured when he was created Baron Meredyth, of Dollarstown in the County of Meath, in the Peerage of the United Kingdom.
After her death in December 1843 he married secondly Maria Georgiana Elizabeth, daughter of Herbert George Jones, in 1860.
Lord Athlumney died in Dover, Kent, in December 1873 and was succeeded by his eldest and only surviving son from his second marriage, James.