In 1827 he entered the Addiscombe Military Seminary and the service of the East India Company. He joined the Bengal Artillery in 1828, and in 1829 arrived in Calcutta. In 1837 he was appointed to the horse artillery and promoted Lieutenant. Two years later, he was appointed Commissary of Ordnance to the Cabul field force. In January 1842, During the First Anglo-Afghan War, Eyre and his family were captured by Akbar Khan. During nearly nine months in captivity, Eyre kept a diary describing his experiences, illustrated by the sketches of other officers and ladies. The manuscript was smuggled out to a friend in British India and was then published in England as Military Operations at Cabul (1843). The Eyre family were rescued by Sir George Pollock in September 1843. In 1844 Eyre was appointed to command the artillery of the new Gwalior contingent. He took part in the Relief of Lucknow, during the Indian Mutiny of 1857. He was promoted Lieutenant-Colonel that year and brevet colonel the following year.
In 1857 he founded Esapore, a colony for destitute families of Portuguese descent. In 1861, Lord Canning selected Eyre to serve on a commission set up to consider amalgamating the Presidency armies of the East India Company with the British Army. In 1863 he was ordered home on sick leave and retired as a major-general.
Finding himself in France during the Franco-Prussian War, Eyre set up an ambulance service under the auspices of the Red Cross. In his later years he spent the winters in Rome and finally died in Aix-les-Bains on 22 September 1881.
- 'The Sikh and European Soldiers of our Indian Forces', The Journal of the Royal United Services Institution, 1867
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