This dataset is a model output from the European Monitoring and Evaluation Programme (EMEP) model applied to the UK (EMEP4UK) driven by Weather and Research Forecast model meteorology (WRF). It provides UK estimates daily averaged atmospheric composition at approximately 5 km grid for the years 2001 to 2015. The data consists of atmospheric composition and deposition values of various pollutants; including PM10, PM2.5, secondary organic aerosols (SOA), elemental carbon (EC), secondary inorganic aerosols (SIA), sulfur dioxide (SO2), ammonia (NH3), nitrogen oxides (NOX) , and ozone (O3). The EMEP model version used here is rv4.17 and the WRF model version is the 3.7.1. This work was supported by the Natural Environment Research Council award number NE/R016429/1 as part of the UK-SCAPE programme delivering National Capability. A version of this dataset is available (https://doi.org/10.5285/ca302d30-7b8b-46ec-90b6-67b79df00c92), run with the latest release of the Atmospheric Chemistry Transport Model EMEP (rv4.36) and with the latest NAEI emissions. The new set of model runs covers an extended time period from 2002 until 2021 and is available in a higher resolution (3 km2 x 3km2). Full details about this dataset can be found at https://doi.org/10.5285/b0545f67-e47c-4077-bf3c-c5ffcd6b72c8