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Abstract Biomass burning smoke aerosols are efficient at attenuating incoming solar radiation. The Layered Atlantic Smoke Interactions with Clouds campaign was conducted from June 2016 to October 2017. The U. S. Department of Energy mobile Atmospheric Radiation Measurement site located on Ascension Island (AMF‐ASI) identified several instances of smoke plume intrusions. Increases in surface and column measurements of aerosol loading were directly related to increases in fine mode fraction, number concentrations of aerosols (N_a), and cloud condensation nuclei (N_CCN). During periods of weak lower tropospheric stability, smoke particles were more likely to be advected downward either by boundary layer turbulence or cloud top entrainment under non‐overcast sky conditions. Backward trajectory analysis illustrated that smoke aerosols reaching the AMF‐ASI site were fine mode, less aged, strongly absorbing, and had shorter boundary layer trajectories while longer boundary layer trajectories denoted mixtures of weakly absorbing smoke and coarse mode marine aerosols. The most polluted smoke cases of August 2016 and 2017 revealed a notable contrast in radiative forcing per unit aerosol optical depth or radiative forcing efficiency (ΔF^eff) at the top of the atmosphere (TOA) and near‐surface (BOA). The weakly (strongly) absorbing 2016 cases exhibited weaker (stronger) ΔF^effat the TOA and BOA suggesting a warming (cooling) effect within the boundary layer. The 2017 cases featured the strongest ΔF^effsuggesting more of a cooling effect at the TOA and BOA due to mixing of fresh smoke with marine aerosols during transport.