This study introduces the concept of “gray carbon,” emphasizing its critical role in carbon sequestration in sewage treatment. By focusing on recalcitrant dissolved organic carbon (RDOC) in sewage effluents and its subsequent transformation in marine environments, we underscore the significant impact of sewage-derived organic carbon on the efficiency of carbon sequestration. Through analysis of carboxylic-rich alicyclic molecules, this study illuminates the convergence in the molecular compositions of RDOC across various aquatic systems. Dark-culture experiments reveal marked variations in the microbial community structures of the aforementioned molecules, indicating that these changes may play an important role in the degradation and subsequent transformation of organic matter in marine environments. These insights lay the groundwork for advancing technologies designed to enhance wastewater alkalinity, which will improve the sustainability of wastewater treatment and preserve marine ecosystems. Enhancing sewage alkalinity can influence microbial processes and chemical equilibria, potentially affecting the formation and accumulation of gray carbon. Further investigation is necessary to understand the potential effect of alkalinity enhancement on the microbial communities and biochemical pathways involved in gray carbon formation. Our findings support the integration of gray carbon strategies into broader carbon neutrality initiatives, providing a scientific and technological blueprint for enhancing global carbon management and mitigating climate change.