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Exploiting a facile way to synthesize low-cost and high-performance oxygen reduction reaction (ORR) catalysts is a core issue in microbial fuel cells (MFCs). Hence, a facile and extensible method has been developed to prepare efficient ORR catalysts by using robust UiO-66 as a precursor, modified with melamine and trithiocyanuric via the impregnation method. Benefiting from the hierarchical structure of UiO-66, the NS@UiO-66 has excellent stability, more active sites and improved mass transfer. Significantly, the half-wave potential and the current density of the NS@UiO-66 are 0.546 V vs. RHE and 6.19 mA cm−2 respectively, which is better than that of benchmark Pt/C in neutral conditions. Furthermore, the power density of MFCs assembled with the NS@UiO-66 catalyst is 318.6 ± 2.15 mW m−2. The density functional theory calculation demonstrates that the reaction barrier can be reduced effectively for accelerating the ORR process through the synergistic effect of N and S. The NS@UiO-66, as an ideal candidate to substitute for the commercial Pt/C counterpart, is expected to promote the scaling-up production and application of MFCs due to low-cost elements doping and facilely synthetic method. [Display omitted] • A facile synthesis way for preparing NS@UiO-66 porous carbon is proposed. • UiO-66 is a stable platform exposing more active sites and boosting mass transfer. • N, S co-doping induces charge redistribution and reduces the activation barrier. • The stable NS@UiO-66 shows great ORR property and application prospects in MFCs. [ABSTRACT FROM AUTHOR]