The datasets of the five Land-offline Model Intercomparison Project (LMIP) experiments using the Chinese Academy of Sciences Land Surface Model (CAS-LSM) of CAS Flexible Global-Ocean-Atmosphere-Land System Model Grid-point version 3 (CAS FGOALS-g3) are presented in this study. These experiments were forced by five global meteorological forcing datasets, which contributed to the framework of the Land Surface Snow and Soil Moisture Model Intercomparison Project (LS3MIP) of CMIP6. These datasets have been released on the Earth System Grid Federation node. In this paper, the basic descriptions of the CAS-LSM and the five LMIP experiments are shown. The performance of the soil moisture, snow, and land-atmosphere energy fluxes was preliminarily validated using satellite-based observations. Results show that their mean states, spatial patterns, and seasonal variations can be reproduced well by the five LMIP simulations. It suggests that these datasets can be used to investigate the evolutionary mechanisms of the global water and energy cycles during the past century.