Climate change mitigation through negative CO2 emissions has been recognized as a crucial strategy to combat global warming. However, its potential effects on terrestrial productivity and agricultural activities remain uncertain. In this study, we utilized large ensemble simulations with an Earth system model of full complexity to investigate the response of Gross Primary Production (GPP) to CO2 forcings. Our findings reveal a significant asymmetry in the GPP response to CO2 ramp-up and symmetric ramp-down model experiments, especially in Europe, suggesting that GPP declines rapidly as CO2 levels decrease. Remarkably, during the CO2 removal period, the North Atlantic Sea surface temperature experienced cooling due to a delayed recovery of the Atlantic Meridional Overturning Circulation (AMOC). This cooling led to precipitation and soil moisture deficits, resulting in a rapid reduction in GPP. This asymmetry in GPP response holds consistent across multi-model simulations. These results underscore the potential implications of delayed recovery in ocean circulation, which could unexpectedly accelerate terrestrial GPP reduction. These insights are crucial for policymakers, aiding them in projecting agricultural activity and formulating targeted GPP control policies specific to the European region.