We present an approach to constrain simulated atmospheric black carbon (BC) using carbon monoxide (CO) observations. The approach uses: (1) the Community Atmosphere Model with Chemistry to simulate the evolution of BC and CO within an ensemble of model simulations; (2) satellite CO retrievals from the MOPITT/Terra instrument to assimilate observed CO into these simulations; (3) the derived sensitivity of BC to CO within these simulations to correct the simulated BC distributions. We demonstrate the performance of this approach through model experiments with and without the BC corrections during the period coinciding with the Intercontinental Chemical Transport Experiment (INTEX‐B). Our results show significant improvements (∼50%) in median BC profiles using constraints from MOPITT, based on comparisons with INTEX‐B measurements. We find that assimilating MOPITT CO provides considerable impact on simulated BC concentrations, especially over source regions. This approach offers an opportunity to augment our current ability to predict BC distributions.