This dataset provides extensive calibration and in-flight performance data for two nucleation mode aerosol size spectrometer (NMASS) instruments utilized in the NASA Atmospheric Tomography Mission (ATom). Each NMASS has five condensation particle counters (CPCs) that detect particles above a different minimum size, determined by the maximum vapor supersaturation encountered by the particles. Operated in parallel, the CPCs provide continuous concentrations of particles in different cumulative size classes between 3 and 60 nm. Knowing the response function of each CPC, numerical inversion techniques were applied to recover size distributions from the continuous concentrations. Data provided include: NMASS counting efficiencies and diameters of calibration aerosols, inverted particle size distributions; comparisons of NMASS and Scanning Mobility Particle Sizer (SMPS) results; and performance at flows, temperatures, and pressures measured by both NMASSs and comparison with Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) concentrations collected on board the NASA DC-8 aircraft during an ATom flight in February 2017.