Mayo is the eldest son of Robert Bourke, 5th Earl of Mayo, and his wife, Anne Charlotte, daughter of the Hon. John Jocelyn. His younger brother, the Hon. Robert Bourke, is also a successful politician. He is educated at Trinity College, Dublin.
After travelling in Russia, Mayo enters parliament for Kildare in 1847, a seat he holds until 1852, and then represents Coleraine from 1852 to 1857 and Cockermouth from 1857 to 1868. He is thrice appointed Chief Secretary for Ireland – in 1852, 1858, and 1866. In 1869 he becomes the fourth Viceroy of India where he is locally often referred to as “Lord Mayo.” He consolidates the frontiers of India and reorganises the country’s finances. He also does much to promote irrigation, railways, forests, and other useful public works. He establishes local boards to solve local problems. During his tenure, the first census takes place in 1872. The European-oriented Mayo College at Ajmer is founded by him for the education of young Indian chiefs, with £70,000 being subscribed by the chiefs themselves.
While visiting the convict settlement at Port Blair in the Andaman Islands in 1872 for the purpose of inspection, he is assassinated by Sher Ali Afridi, an Afridi Pathan convict who uses a knife. His murderer appears to be motivated only by a sense of injustice at his own imprisonment, and has resolved to kill a high-ranking colonial official. Mayo’s body is brought home to Ireland and buried at the medieval ruined church in Johnstown, County Kildare, near his home at Palmerstown House. Afridi is hanged.
In 1873, the newly discovered swallowtail butterfly Papilio mayo from the Andaman Islands is named in his honour. The traditional Irish march Lord Mayo (Tiagharna Mhaighe-eo) is named after him. According to tradition, it is composed by his harper David Murphy to appease Mayo after Murphy angered him.
On August 19, 1875 a statue of Lord Mayo is unveiled in the town of Cockermouth in the centre of the main street. The 800-guinea cost of the statue is raised by public subscription. The statue, carved in Sicilian marble, depicts Lord Mayo in his viceregal garb, and still stands today.
In 2007, a statue of Lord Mayo is unearthed in Jaipur, India, after being buried for six decades. The statue had previously been installed in the premises of Mayo Hospital, currently known as the Mahilya Chikatsalya, Jaipur. The 9-foot-tall cast-iron statue, weighing around 3 tons, was ordered sculpted by the Maharaja Ram Singh ji of Jaipur, as a tribute to Lord Mayo after his assassination. To prevent it from vandalism, the statue is buried in the premises of the Albert Hall Museum of Jaipur at the time of the independence of India. After six decades, the statue is unearthed by the Jaipur Mayo Alumni Chapter on May 29, 2007, and sent to Mayo College, in Ajmer, India, where it is installed. Mayo College in Ajmer already has a full life-size statue of Lord Mayo sculpted in white marble installed in front of its famous Main Building since inception and a marble sculpted bust of him in its School Museum.