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This dataset contains Volatile Organic Compounds (VOC) concentrations taken from a large, population-scale study, which was conducted for a total of 19 weeks during the winter and summer of 2019. VOC concentration data were collected for 39 VOC species across 60 houses in Ashford, United Kingdom. Samples were collected in evacuated stainless-steel canisters over 72 hours using restricted flow inlets. A number of houses were randomly selected to also collect an outdoor sample. Each household, per campaign, was associated with at least three canister IDs and some with an additional outdoor sample. This dataset contains information on all VOCs collected, listing in which season each sample was taken, the associated canister ID and the analytical instrument with which each VOC was measured. Household, demographic, and product use information is available, as is a logbook outlining further sample information.