A continuous decrease in aerosols over the Western North Atlantic Ocean (WNAO) on a decadal timescale provides a long‐term benchmark to evaluate how various natural and anthropogenic processes affect the manifestation of aerosol‐cloud interactions in this region. Furthermore, the WNAO serves as a natural laboratory with diverse aerosol sources, marine boundary layer clouds more variable than those in marine stratocumulus deck regions, and unique flow regimes established by the Gulf Stream and the semi‐permanent Bermuda High. We investigate how satellite‐retrieved macrophysical and microphysical properties of low clouds and the surface shortwave irradiance changed from 2003 to 2020, in tandem with this aerosol decrease. The decadal changes in large‐scale meteorology related to the North Atlantic Oscillation (NAO) are also examined. We find a reduction in low‐cloud optical thickness, accompanied by fewer and larger cloud droplets, yet observe no significant changes in low‐cloud fraction and liquid water path. Despite the reduction in low‐cloud optical thickness together with aerosol decrease, a corresponding increase in the trends of surface shortwave irradiance, also known as surface brightening, is lacking. This absence of brightening is potentially related to concomitant changes found in large‐scale meteorology associated with NAO—Bermuda High strengthening, sea surface warming, and atmospheric moistening— as well as an increase in high‐level cloud fraction that can counteract the surface brightening. Ultimately, our findings suggest that spatial patterns of decadal meteorological variability introduce complexities in the surface cloud radiative effect over the WNAO, thereby complicating the isolation and examination of aerosol‐cloud interactions.