Aerosol optical depth (AOD) is a vital parameter in atmospheric research. Using observations of the Visible Infrared Imaging Radiometer Suite (VIIRS), onboard Suomi National Polar‐orbiting Partnership (Suomi‐NPP) and NOAA‐20 satellites, National Oceanic and Atmospheric Administration (NOAA) produces near‐real time AOD product with high pixel resolution (750 m), wide swath width (3,040 km), and a 16‐day repeat cycle. Here we report the evaluation of the NOAA/VIIRS AOD using a comprehensive aerosol data set, derived from a global‐scale, multi‐seasonal airborne mission, the NASA Atmospheric Tomography Mission (ATom). This data set includes rich physical and chemical information, such as size distributions, chemical compositions, optical properties, and hygroscopicities of major aerosol types, including dust, sea salt, smoke, internally mixed sulfate/nitrate/organics particles (non‐smoke), black carbon, etc. Globally, VIIRS AOD (Suomi‐NPP and NOAA‐20) shows good agreement with the ATom AOD in the moderate to high AOD range (>0.3), with respect to measurement uncertainties (orthogonal distance regression fitting slope: 1.5 ± 0.2 for Suomi‐NPP and 1.6 ± 0.5 for NOAA‐20; correlation coefficient: 0.85 for Suomi‐NPP and 0.73 for NOAA‐20). There is a persistent bias in the low AOD range (<0.3) on the order of 0.03, likely reflecting systematic errors on VIIRS and/or the ATom AOD product. Ångström exponent reported by VIIRS shows excellent agreement with ATom results within expected uncertainties. Given the unique insights revealed by the ATom AOD and aerosol property data set, it is desirable to have ATom‐like comprehensive payloads in future airborne satellite validation programs. Plain Language Summary: Aerosol optical depth (AOD) plays a crucial role in air quality and climate. Satellites have been used to retrieve AOD and other aerosol properties for decades; but satellite retrievals are indirect measurements and need validation using direct measurements. Visible Infrared Imaging Radiometer Suite (VIIRS) is the state‐of‐the‐art instrument that retrieves AOD along with other aerosol properties. In this work, we use the comprehensive aerosol data set from the recent global‐scale, multi‐seasonal ATom field campaign, to evaluate the operational VIIRS AOD product on two satellites (NOAA‐20 and SNPP). This data set includes rich physical and chemical information, such as size distributions, chemical compositions, optical properties, and hygroscopicities of major aerosol types, including dust, sea salt, smoke, internally mixed sulfate/nitrate/organics particles, black carbon, etc. Our analysis shows that the operational VIIRS AOD product is generally accurate and robust. A small bias in the low AOD range has been identified, which could be partially explained by the atmospheric variability, but likely reflects systematic errors on VIIRS and/or the ATom AOD product. Our effort further justifies the global scale suborbital airborne missions (such as HIPPO and ATom) and its unique role in atmospheric/climate research as well as operations. Key Points: National Oceanic and Atmospheric Administration (NOAA)/Visible Infrared Imaging Radiometer Suite (VIIRS) Aerosol optical depth (AOD) (Suomi National Polar‐orbiting Partnership [Suomi‐NPP] and NOAA‐20) generally shows good agreement with the AOD product derived from global‐scale airborne observationsThere is a persistent bias in the low AOD range (<0.3), likely reflecting systematic errors on VIIRS and/or the ATom AOD productComprehensive aerosol observations offer invaluable information for satellite validation and model evaluation [ABSTRACT FROM AUTHOR]