The current study not only characterizes emissions from three coals (bituminous, sub-bituminous, and lignite), but also investigates the use of instrumentation for improved measurement and monitoring techniques that provide real-time, continuous emissions data. Testing was completed using the U.S. EPA’s Multi-Pollutant Control Research Facility, a pilot-scale coal-fired combustor using industry-standard emission control technologies, in Research Triangle Park, North Carolina. Emissions were calculated based on measurements from the flue gas (pre- and post-electrostatic precipitator), to characterize gaseous species (CO, CO2, O2, NOX, SO2, other acid gases, and several organic HAPs) as well as fine and ultrafine particulate (mass, size distribution, number count, elemental carbon, organic carbon, and black carbon). Comparisons of traditional EPA methods to those made via Fourier Transfer Infrared (FTIR) Spectroscopy for CO, NOX, and SO2 are also reported. This dataset is associated with the following publication: Yelverton, T., A. Brashear, D. Nash, E. Brown, C. Singer, P. Kariher, and J. Ryan. Comparison of gaseous and particulate emissions from a pilot-scale combustor using three varieties of coal. FUEL. Elsevier Science BV, Amsterdam, NETHERLANDS, 215: 572-579, (2018).