Microbial fuel cell (MFC) architectural modification is increasingly becoming an important area of research due to the need to improve energy recovery. This study presents a low-cost modification method of the anode that does not require pre-treatment-step involving hazardous chemicals to improve performance. The modification step involves deposition of granular activated carbon (GAC) which is highly conductive and provides a high specific surface area inside a carbon cloth that acts as an anode and as a supporting material. The GAC particle size of 0.6–1.1 mm resulted in an increase in air-cathode MFC performance due to an increase in available surface area of 879.5 m2 g−1 for attachment of cells based on Brunauer, Emmett, and Teller (BET) results, and an increase in the appropriate surface for attachment of cells which was rough based on the scanning electron microscope (SEM) results. On the other hand, although GAC with size of particles of 0.45–0.6 mm had the highest available surface area for attachment of cells, it lacked the appropriate surface for attachment of cells and reduced MFC performance. This means that particle size optimization of GAC is essential since there is a limit to which the particle diameter can be reduced. The utilization of the GAC with the optimized particle size produced an output voltage of 507.5 mV and maximum power output of 1287.7 mW m−3 at current output of 2537.5 mA m−3. This study also showed that there is an economic benefit in modifying carbon cloth using GAC with optimized particle size.