The Triangle Chemical Company Superfund site, in Orange County, Texas, was a chemical mixing and blending facility in the 1970s. According to the Environmental Protection Agency (EPA), poor waste management practices resulted in soil and groundwater contamination and fish-kills in Coon Bayou (U.S. Environmental Protection Agency, 2023). The Five-Year Review of the Triangle Superfund Site indicated groundwater in the upper water-bearing zone might be migrating off-site toward the southwest (U.S. Environmental Protection Agency, 2016). There are concerns regarding potential risks to human health from contaminated soil vapor in existing or future structures in the area. To evaluate the status of volatile organic compound contamination, the U.S. Geological Survey (USGS), in cooperation with the EPA collected passive soil-gas samples, indoor air quality samples, and groundwater-quality samples at the Triangle Chemical Company Superfund Site. In July 2021, passive soil-gas samplers were deployed at 12 locations which collected samples over a 22-day period and indoor air quality samples were collected at two locations immediately southwest of the Site. Samples for 1,4-dioxane were collected from eight monitoring wells at the site on June 1, 2022. To complement and expand on the July 2021 sampling, the USGS deployed passive soil-gas samplers at 22 additional locations over a 14-day period and collected indoor air quality samples at an additional two locations at the site in May 2023. Passive soil-gas and indoor air quality samples collected during these periods were analyzed for a suite of volatile organic compounds (VOCs). This dataset includes the environmental and quality-control data obtained from July 2021 through June 2023 from the passive soil-gas vapor, indoor air quality, and groundwater-quality samples collected at each sample location.