Abstract The roles of organosulfur compounds (OSCs), an important component in organic matter, in brown carbon (BrC) aerosol absorption is often overlooked. Here, the molecular composition of OSCs and its associations with methanol‐soluble BrC (MS‐BrC) absorption during a haze event in North China were revealed using a Fourier transform ion cyclotron resonance mass spectrometry analysis. By combining aggregated boosted tree model and partial least squares regression estimation, our results suggested that OSCs were mainly composed of potential aromatic structures, and the MS‐BrC absorption was closely related to OSCs. Specifically, OSCs contribute a notable 26% of the total potential BrC molecular number and an upper limit of 10.4% of total MS‐BrC absorption. Furthermore, we found that OSCs were mainly influenced by coal combustion, and the potential desulfurization reactions showed associations with the variations of MS‐BrC absorption. Since the residential coal combustion (an important primary source of OSs) was the major energy in North China, our research underscores the potential of aromatic OSCs as tracers for assessing the impact of fossil fuel combustion on BrC and highlights the important atmospheric influences of OSCs (e.g., light absorption and health), which need more works to uncover the origins, fates, and environmental effects of OSCs.