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Aerosol-cloud interactions (ACIs) are vital for regulating Earth’s climate by influencing energy and water cycles. Yet, effects of ACI bear large uncertainties, evidenced by systematic discrepancies between observed and modeled estimates. This study quantifies a major bias in ACI determinations, stemming from conventional surface or space measurements that fail to capture aerosol at the cloud level unless the cloud is coupled with land surface. We introduce an advanced approach to determine radiative forcing of ACI by accounting for cloud-surface coupling. By integrating field observations, satellite data, and model simulations, this approach reveals a drastic alteration in aerosol vertical transport and ACI effects caused by cloud coupling. In coupled regimes, aerosols enhance cloud droplet number concentration across the boundary layer more homogeneously than in decoupled conditions, under which aerosols from the free atmosphere predominantly affect cloud properties, leading to marked cooling effects. Our findings spotlight cloud-surface coupling as a key factor for ACI quantification, hinting at potential underassessments in traditional estimates.