Recent lithogeochemical studies by accurate analytical techniques (e.g., instrumental and radiochemical neutron-activation analyses) have been used to explore the possibility of using gold distribution in the research for new gold deposits; these show that anomalous gold distribution occurs in some parts of the Val-d'Or Formation in the Val-d'Or mining district of Quebec. Gold lithogeochemistry in the Val-d'Or Formation has shown that it is possible to distinguish: (i) background values (1.4–3.5 ppb Au); (ii) zones of primarily anomalous gold values around the Lamaque–Sigma mines (median: 15 ppb Au); (iii) enrichment halos around gold orebodies (median: 70 ppb Au); and (iv) secondary gold enrichment in shear zones. We conclude that the Val-d'Or Formation is auriferous, i.e., anomalously rich in gold at least in some of its parts and contains the Lamaque – Sigma gold mines, representing 68% of the total gold production in the district. The Val-d'Or Formation is part of a central volcanic complex within an island-arc system. The centre of this complex is located in the main Lamaque plug, and this environment may be compared to high-temperature active geothermal systems that are commonly responsible for the formation of epithermal gold deposits. Gold mineralization at Sigma and Lamaque is considered to be related to a late hydrothermal phase or a retrograde phase of regional metamorphism. For the formation of the gold deposits, two distinct and successive events are postulated: (i) a gold-rich synvolcanic geothermal activity and (ii) a late remobilisation from the host rocks followed by deposition of gold ore within favourable structures.