The light-absorbing chemical components of atmospheric organic aerosols are commonly referred to as Brown Carbon (BrC), reflecting the characteristic yellowish to brown appearance of aerosol. BrC is a highly complex mixture of organic compounds with diverse compositions and variable optical properties of its individual chromophores. BrC significantly influences the radiative budget of the climate and contributes to adverse air pollution effects such as reduced visibility and the presence of inhalable pollutants and irritants. However, a fundamental understanding of the sources, formation, and transformation (aging effects) of BrC remains incomplete. This gap in knowledge necessitates advanced chemical characterization of individual aerosol components and the correlation of their composition with optical properties. Over the past decade, a multi-modal analytical platform composed of high-performance liquid chromatography with a photodiode array UV-vis detector and high-resolution mass spectrometry has been extensively used for the untargeted analysis of BrC components in complex mixtures of atmospheric organic aerosols and their laboratory proxies. This method separates solvent-extractable BrC compounds into distinct fractions, each characterized by specific retention times, UV-vis absorption spectra, and elemental compositions, offering comprehensive molecular insights into BrC components. In this review, we highlight the application of this platform in analyzing both real-world aerosol samples and laboratory-generated proxies. These studies have identified composition-specific sources and transformations of BrC, advancing our understanding of these complex atmospheric mixtures. Atmospheric humic-like substances (HULIS), formed through cloud processing of wildfire smoke and the oligomerization of water-soluble organics, are key contributors to BrC. Additional HULIS originate from fossil fuel combustion, biogenic, and marine emissions. Key BrC chromophores include nitroaromatics, imidazoles, N-heterocycles, polyaromatic hydrocarbons, quinones, and others. Aging processes, including photolysis and multiphase reactions, can significantly alter BrC optical properties by generating new chromophores or degrading existing ones. The fundamental knowledge gained from these investigations is essential for assessing BrC optical properties. Additionally, it provides practical composition metrics necessary to inform and improve future atmospheric models, enabling more accurate predictions of BrC behavior and its impact on climate and air quality.