AbstractIn this work, we apply the GFDL Earth System Model (GFDL‐ESM4.1) to explore the climate responses to a stratospheric aerosol injection (SAI) scenario that aims to restrict global warming to 2.0°C above pre‐industrial levels (1850–1900) under the CMIP6 overshoot scenario (SSP5‐34‐OS). Simulations of this SAI scenario with the CESM Whole Atmosphere Community Climate Model (CESM2‐WACCM6) showed nearly unchanged interhemispheric and pole‐to‐Equator surface temperature gradients relative to present‐day conditions around 2020, and reduced global impacts, such as heatwaves, sea ice melting, and shifting precipitation patterns (Tilmes et al., 2020, https://doi.org/10.5194/esd‐11‐579‐2020). However, model structural uncertainties can lead to varying climate projections under the same forcing. Implementing identical stratospheric aerosol radiative properties in GFDL‐ESM4.1, which has a much lower Effective Climate Sensitivity compared to CESM2‐WACCM6, resulted in a decrease in global‐mean surface temperature by more than 1.5°C and a corresponding reduction in precipitation responses. Two major reasons contribute to the different temperature response between the two models: first, GFDL‐ESM4.1 has less warming in the SSP534‐OS scenario; second, GFDL‐ESM4.1 has shown more pronounced cooling in response to the same stratospheric AOD perturbation. Notably, the Southern Hemisphere experiences substantial cooling compared to the Northern Hemisphere, accompanied by a northward shift of the Intertropical Convergence Zone (ITCZ). Furthermore, our analysis reveals that spatially heterogeneous forcing within the SAI scenario results in diverse climate feedback parameters in the GFDL‐ESM4.1 model, through varying surface warming/cooling patterns. This research highlights the importance of considering model structural uncertainties and forcing spatial patterns for a comprehensive evaluation of future scenarios and geoengineering strategies.