A large decrease in the land surface albedo of the Loess Plateau was observed from 2000 to 2010, as measured using satellite imagery. In particular, ecological restoration program regions experienced a decrease in peak season land surface albedo exceeding 0.05. In this study, we examined the spatial and temporal patterns of variation during the peak season albedo in the Loess Plateau and analyzed its relationships with changes of anthropogenic and natural factors at the pixel level. Our analysis revealed that increasing grassland coverage due to returning rangeland to grassland could lead to a maximum albedo decrease of 0.030 in peak season. This result highlighted the human-induced land use change in driving the decreasing albedo on an annual scale. There was no significant correlation between precipitation change and albedo reduction. Precipitation could influence the spatial pattern of albedo in drought years by influencing the natural vegetation water requirement. However, the role of precipitation was not obvious in the ecological restoration program regions. This article demonstrates the substantial role that land use change could play in regional-scale albedo change and climate. Finally, some implications for the radiative forcing of land use change are discussed.