Aerosol measurements during the DOE ARM Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign were used to quantify the differences between clean and smoky cloud condensation nuclei (CCN) budgets. Accumulation‐mode particles accounted for ∼70% of CCN at supersaturations <0.3% in clean and smoky conditions. Aitken‐mode particles contributed <20% and sea‐spray‐mode particles <10% at supersaturations <0.3%, but at supersaturations >0.3% Aitken particles contributions increased to 30%–40% of clean CCN. For clean conditions, the Hoppel minimum diameter was correlated to the accumulation‐mode number concentration, indicating aerosol‐correlated cloud activation was controlling the lower diameter cutoff for which particles serve as CCN. For smoky conditions, the contributions of Aitken particles increase and the correlation of cloud activation to accumulation‐mode particles is masked by the lower‐hygroscopicity smoke. These results provide the first multi‐month in situ quantitative constraints on the role of aerosol number size distributions in controlling cloud activation in the tropical Atlantic boundary layer. Plain Language Summary Tiny airborne particles provide the “seeds” on which cloud droplets form, and clouds are in turn important for regulating climate around the world. The small number of measurements characterizing these particles in conditions that are not affected by man‐made emissions make it difficult to represent these cloud processes in computer models that compare current climate to pre‐industrial conditions. Aerosol measurements collected for 17 months on an isolated island in the tropical Atlantic Ocean show how the size and number of particles affect cloud characteristics. The long timescale and wide range from very clean to very smoky aerosol conditions revealed not only differences in the particles that activate in clouds but also in the mechanisms that control that droplet formation process. In clean air, the size required to form a cloud droplet is influenced by the number of particles, as well as how quickly particles take up water during growth in cloud. However, in smoky air, the larger number and size of particles mean that cloud activation processes are less affected by the number of particles that take up water. Key Points Clean cloud condensation nuclei (CCN) at <0.3% supersaturation were ∼70% accumulation, <10% sea spray, and <20% Aitken mode particles Hoppel minimum diameters correlated to accumulation‐mode particles showing aerosol‐correlated activation for clean conditions (<400 cm−3) Smoky accumulation‐mode particles were 30 nm larger and had 15%–30% more CCN, which dampened correlations to cloud activation