Natural emissions of air pollutants from the surface play major roles in air quality and climate change. In particular, nitrogen oxides (NOx) emitted from soils contribute ~15% of global NOx emissions, sea salt aerosols are a major player in the climate and chemistry of the marine atmosphere, and biogenic emissions are the dominant source of non-methane volatile organic compounds at the global scale. These natural emissions are often estimated using nonlinear parameterizations, which are sensitive to the horizontal resolutions of inputted meteorological and ancillary data. Here we use the HEMCO model to compute these emissions worldwide at horizontal resolutions of 0.5° lat. × 0.625° lon. for 1980-2017 and 0.25° lat. × 0.3125° lon. for 2014-2017. We further offer the respective emissions at lower resolutions, which can be used to evaluate the impacts of resolution on estimated global and regional emissions. Our long-term high-resolution emission datasets offer useful information to study natural pollution sources and their impacts on air quality, climate, and the carbon cycle.