We explore the extent to which chemistry-aerosol-climate coupling influences predictions of future ozone and aerosols as well as future climate using the Goddard Institute for Space Studies (GISS) general circulation model II' with on-line simulation of tropospheric ozone-NOx-hydrocarbon chemistry and sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon aerosols. Based on IPCC scenario A2, year 2100 ozone, aerosols, and climate simulated with full chemistry-aerosol-climate coupling are compared with those simulated from a stepwise approach. In the stepwise method year 2100 ozone and aerosols are first simulated using present-day climate and year 2100 emissions (denoted as simulation CHEM2100sw) and year 2100 climate is then predicted using offline monthly fields of O3 and aerosols from CHEM2100sw (denoted as simulation CLIM2100sw). The fully coupled chemistry-aerosol-climate simulation predicts a 15% lower global burden of O3 for year 2100 than the simulation CHEM2100sw which does not account for future changes in climate. Relative to CHEM2100sw, year 2100 column burdens of all aerosols in the fully coupled simulation exhibit reductions of 10–20 mg m−2 in DJF and up to 10 mg m−2 in JJA in mid to high latitudes in the Northern Hemisphere, reductions of up to 20 mg m−2 over the eastern United States, northeastern China, and Europe in DJF, and increases of 30–50 mg m−2 over populated and biomass burning areas in JJA. As a result, relative to year 2100 climate simulated from CLIM2100sw, full chemistry-aerosol-climate coupling leads to a stronger net global warming by greenhouse gases, tropospheric ozone and aerosols in year 2100, with a global and annual mean surface air temperature higher by 0.42 K. For simulation of year 2100 aerosols, we conclude that it is important to consider the positive feedback between future aerosol direct radiative forcing and future aerosol concentrations; increased aerosol concentrations lead to reductions in convection and precipitation (or wet deposition of aerosols), further increasing lower tropospheric aerosol concentrations.