Aerosols and meteorological clouds represent major sources of uncertainty in understanding past and future climate variability. Each phenomenon is both influenced by –and influences via radiative forcing– the climate system. Thus, quantifying historical changes in aerosols and clouds, determining the underlying causes of such variability, and uncovering the manner by which aerosol and cloud radiative forcing alters the evolution of the climate-system are of utmost importance. Our research elucidates such questions via analysis of historical data, numerical experimentation, and development of theoretical frameworks for understanding how aerosols, clouds, and climate co-vary over a range of spatial and temporal scales.