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Algal biocathodes in microbial fuel cells (MFCs) are becoming more attractive as an effective and potential solution to overcome the limiting aspects of oxygen (O₂) reduction and other limitations caused by abiotic and general biocathodes in MFC. The presence of algae in biocathode of MFC generates O₂ via photosynthesis and aids in the enhancement of MFC performance in an environmentally sustainable way by reducing the overpotentials caused by various losses. The applications of algal biocathodes in MFCs require knowledge at both engineering and scientific fields for efficient carbon dioxide sequestration, wastewater treatment (nutrient uptake), in situ O₂ generation, and biomass for biofuel, biofertilizer, and other value-added products generation. The significance and role of algal biocathodes during the MFC operation have been detailed in the present chapter.