This dataset contains high‑frequency measurements of volatile organic compounds (VOCs) and their surface-atmosphere fluxes collected at an urban site in Old Delhi, India. The measurements capture both VOC concentrations and bidirectional fluxes, allowing users to investigate emission and deposition processes within a densely populated megacity. Data were collected between 9 October and 23 November 2018 at a 25‑metre tower located at the Indira Gandhi Delhi Technical University for Women (IGDTUW), within an urban footprint influenced by traffic, domestic combustion, industrial activity, evaporative sources and occasional pyrotechnic events. The dataset includes 5 Hz VOC concentration time series from a Proton‑Transfer‑Reaction Time‑of‑Flight Mass Spectrometer (PTR‑QiTOF‑MS), co‑located high‑frequency wind measurements from a sonic anemometer, Virtual Eddy Accumulation (VEA) updraft and downdraft concentration data, and fluxes derived using both standard eddy‑covariance and numerical VEA methods. It also provides Positive Matrix Factorisation (PMF) outputs, including source‑resolved VOC factors and their associated fluxes. Relevant meteorological variables and supporting chemical indicators are included to aid interpretation. These data allow users to assess local emission sources, bidirectional VOC exchange, diurnal patterns, and chemical drivers relevant to ozone formation and atmospheric reactivity. The dataset is suitable for researchers studying urban air pollution, VOC source apportionment, atmospheric chemistry and model development. The work was supported by the Natural Environment Research Council (NE/P016502/1, NE/P016472/1, NE/L002558/1 and NE/R000131/1) and the Earth System Science Organization, Ministry of Earth Sciences (Government of India, MoES/16/19/2017-APHH) Full details about this dataset can be found at https://doi.org/10.5285/9fdea71b-7719-4c2f-8ddf-7311ecdb4418