The Rb/Sr ratio of lake sediments has been demonstrated to be a potential indicator of chemical weathering by increasing work. However, Rb and Sr in lake sediments are derived from both chemical weathering and physical erosion. Rb and Sr of different forms in lake sediments may record different environmental processes and information. In this study, the variation patterns of Rb and Sr of different forms in sediments of Daihai Lake were investigated. The results show that Rb and Sr of different forms display noticeably different variation patterns due to their different sources and associated environmental processes. Using the Rb/Sr ratios of bulk lake sediments to reflect chemical weathering is not accurate. The non-residual Sr of the sediments without detrital carbonates, representing the Sr leached from the catchment, can be used as an index of chemical weathering because the weathering of Sr minerals is very sensitive to climate change, and the non-residual Sr content of the sediment is determined more by Sr2 + influx than by the physicochemical conditions of lake water. The correspondence between the non-residual Sr and TIC/TOC in Daihai Lake also indicates that the non-residual Sr of the sediments is a good indicator of chemical weathering in the catchment.