The 2014–15 Holuhraun eruption created a vast aerosol plume that acted as a natural experiment to assess how well climate models capture changes in cloud properties due to increased aerosol. We find that climate models represent the observed shift to smaller, more numerous cloud droplets well. However, climate models diverge in their aerosol-induced changes to large-scale cloud properties, particularly cloud liquid water content. Our study shows that Holuhraun had a cooling effect on the Earth.