Land surface processes are rarely studied in Detection and Attribution Model Inter-comparison Project (DAMIP) experiments on climate change. We analyzed a CMIP6 DAMIP historical experiment by using multi-linear regression (MLRM) and analysis of variance methods. We focused on energy and water budgets, including gross primary productivity (GPP). In MLRM, we estimated each forcing’s contribution and identified the role of natural forcing, which is usually ignored. Contributions of the forcing factors varied by region, and high-ranked variables such as net radiation could receive multiple influences. Greenhouse gases (GHG) accelerated energy and water cycles over the global land surface, including evapotranspiration, runoff, GPP, and water-use efficiency. Aerosol (AER) forcing displayed the opposite characteristics, and natural forcing accounted for short-term changes. A long-term analysis of total soil moisture and water budget indicated that as the AER increases, the available water on the global land increases continuously. In the recent past, an increase in net radiation (i.e., a lowered AER) reduced surface moisture and hastened surface water cycle (GHG effect). The results imply that aerosol emission and its counterbalance to GHG are essential to most land surface processes. The exception to this is GPP, which was overdominated by GHG effects.