A new high-resolution global tropospheric aerosol dataset with monthly resolution is generated using version 4 of the Community Atmosphere Model (CAM4) coupled to a bulk aerosol model and forced with recent estimates of surface emissions for the period 1961–2000 to identify tropospheric aerosol-induced interannual climate variations. The surface emissions dataset is constructed from phase 5 of the Coupled Model Intercomparison Project (CMIP5) decadal-resolution surface emissions dataset to include reanalysis of tropospheric chemical composition [40-yr Reanalysis of Tropospheric Chemical Composition (RETRO)] wildfire monthly emissions data. A four-member ensemble run is conducted using the spectral configuration of CAM4, forced with the new tropospheric aerosol dataset and prescribed with observed sea surface temperature, sea ice, and greenhouse gases. CAM4 only simulates the direct and semidirect effects of aerosols on the climate. The simulations reveal that variations in tropospheric aerosol levels can induce significant regional climate variability on the interannual time scales. Regression analyses over tropical Atlantic and Africa suggest that increasing dust aerosols can cool the North African landmass and shift convection southward from West Africa into the Gulf of Guinea in the spring season. Further, it is found that carbonaceous aerosols emanating from the southwestern African savannas can significantly cool the region and increase the marine stratocumulus cloud cover over the southeast tropical Atlantic Ocean by aerosol-induced diabatic heating of the free troposphere above the low clouds. Experiments conducted with CAM4 coupled to a slab ocean model suggest that present-day aerosols can cool the tropical North Atlantic and shift the intertropical convergence zone southward and can reduce the ocean mixed layer temperature beneath the increased marine stratocumulus clouds in the southeastern tropical Atlantic.