This study investigates dimming and brightening of surface solar radiation (SSR) during 1961–2005 in China as well as its relationships to total cloud cover (TCC). This is inferred from daily ground-based observational records at 45 pyranometer stations. A statistical method is introduced to study contributions of changes in the frequency of TCC categories and their atmospheric transparency to the secular SSR trend. The surface records suggest a renewed dimming beyond 2000 in North China after the stabilization in the 1990s; however, a slight brightening appears beyond 2000 in South China. Inter-annual variability of SSR is negatively correlated with that of TCC, but there is a positive correlation between decadal variability of SSR and TCC in most cases. The dimming during 1961–1990 is exclusively attributable to decreased atmospheric transparency, a portion of which is offset by TCC frequency changes in Northeast and Southwest China. The dimming during 1961–1990 in Northwest and Southeast China primarily results from decreased atmospheric transparency under all sky conditions and the percentage of dimming stemming from TCC frequency changes is 11% in Northwest and 2% in Southeast China. Decreased atmospheric transparencies during 1991–2005 in North China in most cases lead to the dimming. TCC frequency changes also contribute to the dimming during this period in North China. This feature is more pronounced in summer and winter when TCC frequency changes can account for more than 80% of dimming. In South China, increased atmospheric transparencies lead to the brightening during 1991–2005. A substantial contribution by TCC frequency changes to the brightening is also evident in spring and autumn.