Absorption aerosol optical depth (AAOD) measurements made by sun-sky photometers are currently the only constraint available for estimates of the global radiative forcing of black carbon (BC), but their validation studies are limited. In this paper, we report the first attempt to compare AAODs derived from single-particle soot photometer (SP2) and ground-based sun-sky photometer (sky radiometer, SKYNET) measurements. During the Aerosol Radiative Forcing in East Asia (A-FORCE) experiments, BC size distribution and mixing state vertical profiles were measured using an SP2 on board a research aircraft near the Fukue Observatory (32.8°N, 128.7°E) over the East China Sea in spring 2009 and late winter 2013. The aerosol extinction coefficients (bext) and single scattering albedo (SSA) at 500 nm were calculated based on aerosol size distribution and detailed BC mixing state information. The calculated aerosol optical depth (AOD) agreed well with the sky radiometer measurements (2 ± 6%) when dust loadings were low (lidar-derived nonspherical particle contribution to AOD less than 20%). However, under these low-dust conditions, the AAODs obtained from sky radiometer measurements were only half of the in situ estimates. When dust loadings were high, the sky radiometer measurements showed systematically higher AAODs even when all coarse particles were assumed to be dust for in situ measurements. These results indicate that there are considerable uncertainties in AAOD measurements. Uncertainties in the BC refractive index, optical calculations from in situ data, and sky radiometer retrieval analyses are discussed.