Reducing methane (CH4) emissions is an attractive option for jointly addressing climate and ozone (O3) air quality goals. With multidecadal full-chemistry transient simulations in the MOZART-2 tropospheric chemistry model, we show that tropospheric O3 responds approximately linearly to changes in CH4 emissions over a range of anthropogenic emissions from 0–430 Tg CH4 a−1 (0.11–0.16 Tg tropospheric O3 or ∼11–15 ppt global mean surface O3 decrease per Tg a−1 CH4 reduced). We find that neither the air quality nor climate benefits depend strongly on the location of the CH4 emission reductions, implying that the lowest cost emission controls can be targeted. With a series of future (2005–2030) transient simulations, we demonstrate that cost-effective CH4 controls would offset the positive climate forcing from CH4 and O3 that would otherwise occur (from increases in NOx and CH4 emissions in the baseline scenario) and improve O3 air quality. We estimate that anthropogenic CH4 contributes 0.7 Wm−2 to climate forcing and ∼4 ppb to surface O3 in 2030 under the baseline scenario. Although the response of surface O3 to CH4 is relatively uniform spatially compared to that from other O3 precursors, it is strongest in regions where surface air mixes frequently with the free troposphere and where the local O3 formation regime is NOx-saturated. In the model, CH4 oxidation within the boundary layer (below ∼2.5 km) contributes more to surface O3 than CH4 oxidation in the free troposphere. In NOx-saturated regions, the surface O3 sensitivity to CH4 can be twice that of the global mean, with >70% of this sensitivity resulting from boundary layer oxidation of CH4. Accurately representing the NOx distribution is thus crucial for quantifying the O3 sensitivity to CH4.