As an important fraction of light-absorbing particles, black carbon (BC) has a significant warming effect, despite accounting for a small proportion of total aerosols. A comprehensive investigation was conducted on the characteristics of atmospheric aerosols and BC particles over Wuhan, China. Mass concentration, optical properties, and radiative forcing of total aerosols and BC were estimated using multi-source observation data. Results showed that the BC concentration monthly mean varied from 2.19 to 5.33 μg m−3. The BC aerosol optical depth (AOD) maximum monthly mean (0.026) occurred in winter, whereas the maximum total AOD (1.75) occurred in summer. Under polluted-air conditions, both aerosol radiative forcing (ARF) and BC radiative forcing (BCRF) at the bottom of the atmosphere (BOA) were strongest in summer, with values of −83.01 and −11.22 W m−2, respectively. In summer, ARF at BOA on polluted-air days was more than two-fold that on clean-air days. In addition, compared with clean-air days, BCRF at BOA on polluted-air days was increased by 76% and 73% in summer and winter, respectively. The results indicate an important influence of particulate air pollution on ARF and BCRF. Furthermore, the average contribution of BCRF to ARF was 13.8%, even though the proportion of BC in PM2.5 was only 5.1%.