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• A critical review of photocatalytic and biodesulphurization methods is presented. • The mechanism of coal desulphurization is critically discussed. • Challenges faced in photocatalytic desulphurization are highlighted. • A hybrid system for biodesulphurization in synergy with CO 2 mitigation is proposed. • Cost analysis of simultaneous biodesulphurization and CO 2 consumption is reviewed. Developing efficient methods for deep desulphurization of commercial fuel is of utmost importance due to the environmental impact of sulphur and stringent government regulations for sulphur-free fuel. This review highlighted the significance of photo-assisted biocatalytic desulphurization of coal and introduced novel strategies that combine coal desulphurization with CO 2 mitigation. The interactions between microbes and the mechanisms underlying the biodesulphurization of coal were thoroughly discussed. Furthermore, the effect of coal structure and porosity on the desulphurization of inorganic sulphur was analyzed. It is acknowledged that achieving high catalytic efficiency and stability of the catalyst during photocatalytic desulphurization remains a challenge. The review also identified microbial species that are most suitable for simultaneous biodesulphurization and CO 2 mitigation, taking into account their mutualistic growth patterns. Besides, the mechanisms and cost-benefit analysis of coal biodesulphurization with high CO 2 consumption by bacterial communities in a hybrid system were further examined. The insights provided in this review can offer a comprehensive understanding of the design of a hybrid system capable of self-capturing CO 2 from polluted atmospheres and utilizing it in a reactor for cost-effective coal biodesulphurization, which holds great potential for combating smog and global warming. [ABSTRACT FROM AUTHOR]