The NOAA Lockheed Orion WP-3D aircraft intercepted a forest fire plume over Utah on 19 May 2002 during the Intercontinental Transport and Chemical Transformation (ITCT) mission. Large enhancements in acetonitrile (CH3CN), carbon monoxide (CO) and particle number were measured during the fire plume interception. In the 100 s plume crossing, the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument acquired 202 positive mass spectra from ionizing single particles in the 0.2–5 μm size range. These particles contained carbon, potassium, organics, and ammonium ions. No pure soot particles were sampled directly from the plume. By characterizing these particle mass spectra, a qualitative biomass-burning particle signature was developed that was then used to identify biomass-burning particles throughout ITCT. The analysis was extended to identify biomass-burning particles in four other missions, without the benefit of gas-phase biomass-burning tracers. During ITCT, approximately 33% of the particles sampled in the North American troposphere and 37% of the particles transported from Asia, not influenced by North American sources, were identified as biomass-burning particles. During the WB-57 Aerosol Mission (WAM), Atmospheric Chemistry of Combustion Emissions near the Tropopause (ACCENT) and ACCENT 2000 missions, 7% of stratospheric particles were identified as biomass-burning particles. During the Cirrus Regional Study of Tropical Anvils and Cirrus Layers – Florida Area Cirrus Experiment (CRYSTAL-FACE) this percentage increased to 52% because the regional stratosphere was strongly affected by an active fire season.