In 1827, while stationed at Agra, he and a colleague deserted and traveled through parts of the Punjab that were under British control at that time. At Ahmadpur, they were rescued by Josiah Harlan and commissioned as mounted orderlies in his expedition to overthrow the regime in Kabul, Afghanistan. Not long afterward, near Dera Ghazi Khan, he deserted Harlan. Between 1833 and 1838, Masson excavated over 50 Buddhist sites around Kabul and Jalalabad in south-eastern Afghanistan, amassing a large collection of small objects and many coins, principally from the site at Bagram, north of Kabul. From 1827, when he deserted, to his return to England in 1842, it is estimated that Masson collected around 47,000 coins. Masson was the first European to see the ruins of Harappa, described and illustrated in his book Narrative of Various Journeys in Balochistan, Afghanistan and The Punjab. He also visited the North-West Frontier Province and Balochistan, serving as an agent of the East India Company. In the 1930s, the found unexpected evidence of an earlier European visitor scribbled in one of the caves above the 55 m Buddha at Bamiyan. This stated:
Through his wide-ranging travels, Masson built up an extraordinary collection of artefacts largely from the modern states of Afghanistan and Pakistan. Numbering about 9,000 objects, they are now held by the British Museum. The Masson Project is led by Dr Elizabeth Errington, and aims to publish Masson's collection. Publications so far include: Two major catalogues
Charles Masson and the Buddhist Sites of Afghanistan: Explorations, Excavations, Collections 1832-1835, by Elizabeth Errington, British Museum Research Publication 215.
The Charles Masson Archive: British Library, British Museum and Other Documents Relating to the 1832–1838 Masson Collection from Afghanistan, by Elizabeth Errington, assisted by Piers Baker, Kirstin Leighton-Boyce and Wannaporn Kay Rienjang, British Museum Research Publication 216.
Shorter articles
E. Errington and V.S. Curtis, From Persepolisto the Punjab. Exploring the Past in Iran, Afghanistan and Pakistan, passim.
E. Errington, ‘“Boots”, “female idols” and disembodied heads’, Journal of Inner Asian Art and Archaeology I, pp. 89-96
E. Errington, ‘Ancient Afghanistan through the eyes of Charles Masson: the Masson Project at the British Museum’, International Institute for Asian Studies Newsletter, pp. 8-9
E. Errington, ‘The collections of Charles Masson ’, Circle of Inner Asian Art Newsletter 15, pp. 29-30
E. Errington, ‘Discovering ancient Afghanistan, The Masson Collection’, Minerva 13/6, pp. 53-5
E. Errington, ‘Discovering ancient Afghanistan’, British Museum Magazine 44, p. 8
E. Errington, ‘Charles Masson and Begram’, Topoi 11/1, pp. 357-409
E. Errington, ‘Rediscovering the collections of Charles Masson’, in M. Alram and D. E. Klimburg-Salter Coins, Art and Chronology. Essays on the pre-Islamic History of the Indo-Iranian Borderlands, pp. 207-37