The Loess Plateau (LP) ecosystems are expected to play an important role in achieving the national carbon neutrality goals. However, significant uncertainty remains in assessing the spatiotemporal dynamics of carbon sequestration rates (CSRs) in regional terrestrial ecosystems. Here, we integrated large amounts of field-plot data and models (forest carbon sequestration model and machine learning models) to systematically explore the CSR of terrestrial ecosystems over the LP from 1980 to 2060 under three climate scenarios. Results showed that an increase of 2.62 +/- 0.43 Pg C for terrestrial ecosystems over the LP during 1980-2060, with 1.98 +/- 0.31 Pg C and 0.64 +/- 0.13 Pg C in vegetation and soil, respectively, representing an increase of 54.60%. The CSR of forests, shrublands, grasslands, and croplands over the LP were estimated to be 36.63 +/- 6.96, 0.09 +/- 0.01,-7.74 +/- 1.13, and 3.81 +/- 0.66 Tg C yr-1, respectively. Between 1980 and 2060, the ecosystem CSR (ECSR) over the LP ranged from 9.62 to 64.45 Tg C yr-1, with an average of 32.78 +/- 6.79 Tg C yr-1. The ECSR will be peaking during 2040-2050 before decreasing. Our findings provide comprehensive picture of the spatiotemporal dynamic trajectory of CSR over the LP and can be used to inform future policymaking to achieve regional carbon neutrality.