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Nevill went to Sri Lanka in 1865, as a Private Secretary to the Chief Justice. From 1869 to 1897 he followed a career in the British Civil Service, which led to his appointment as District Judge of Batticaloa. In 1897 he sailed for France, but died soon after.

Nevill was a pioneer student of the origin and development of Sinhala, the main language of Sri Lanka, and of the dialects of the Veddhas, Rodiyas, and Vanniyas. He was the founder and a major contributor of the scholarly journal The Taprobanian, and of the Kandyan Society of Arts. His interests and publications were extremely broad, covering anthropology, archaeology, botany, ethnology, folklore, geography, geology, history, mythology, palaeography, philology, and zoology.

During his 32 years in Sri Lanka, Nevill assembled a collection of 2,227 prose and verse manuscripts, mostly in Sinhala, Malayalam, Tamil, and Pali, now kept at the British Library. He produced a critical catalog of the collection, in two volumes, but died before it was published. A more detailed description, in seven volumes, was eventually prepared by K. D. Somadasa and published by the Library.

One of these manuscripts is the Sri Lanka Portuguese Creole Manuscript, the earliest text of significant length in the Indo-Portuguese creole spoken by the Burghers and Kaffirs communities of Sri Lanka.

Many objects collected by Nevill in Sri Lanka were acquired by the British Museum.