This work studied the performance of a laboratory-scale microbial fuel cell (MFC) using a bioanode that consisted of treated clinoptilolite fine powder coated onto graphite felt (TC-MGF). The results were compared with another similar MFC that used a bare graphite felt (BGF) bioanode. The anode surfaces provided active sites for the adhesion of the bacterial consortium (NAR-2) and the biodegradation of mono azo dye C.I. Acid Red 27. As a result, bioelectricity was generated in both MFCs. A 98% decolourisation rate was achieved using the TC-MGF bioanode under a fed-batch operation mode. Maximum power densities for BGF and TC-MGF bioanodes were 458.8 ± 5.0 and 940.3 ± 4.2 mW m-2, respectively. GC-MS analyses showed that the dye was readily degraded in the presence of the TC-MGF bioanode. The MFC using the TC-MGF bioanode showed a stable biofilm with no biomass leached out for more than 300 h operation. In general, MFC performance was substantially improved by the fabricated TC-MGF bioanode. It was also found that the TC-MGF bioanode with the stable biofilm presented the nature of exopolysaccharide (EPS) structure, which is suitable for the biodegradation of the azo dye. In fact, the EPS facilitated the shuttling of electrons to the bioanode for the generation of bioelectricity.