In this study, multiple remote sensing data were used to quantitatively evaluate the contributions of surface water, soil moisture and groundwater to terrestrial water storage (TWS) changes in five groundwater resources zones of Inner Mongolia (GW_I, GW_II, GW_III, GW_IV and GW_V), China. The results showed that TWS increased at the rate of 2.14 mm/a for GW_I, while it decreased at the rate of 4.62 mm/a, 5.89 mm/a, 2.79 mm/a and 2.62 mm/a for GW_II, GW_III, GW_IV and GW_V during 2003–2021. Inner Mongolia experienced a widespread soil moisture increase with the rate of 4.17 mm/a, 2.13 mm/a, 1.20 mm/a, 0.25 mm/a and 1.36 mm/a for the five regions, respectively. Significant decreases were detected for regional groundwater storage (GWS) with the rate of 2.21 mm/a, 6.76 mm/a, 6.87 mm/a, 3.01 mm/a, and 4.14 mm/a, respectively. Soil moisture was the major contributor to TWS changes in GW_I, which accounted 58% of the total TWS changes. Groundwater was the greatest contributor to TWS changes in other four regions, especially GWS changes, which accounted for 76% TWS changes in GW_IV. In addition, this study found that the role of surface water was notable for calculating regional GWS changes.