Although biomass-derived carbon and metal-organic-framework-based materials have been widely studied, their integration as self-supported cathodes for sediment microbial fuel cells remains limited. This study investigated carbonized wood cathodes functionalized with cobalt- and nickel-based metal-organic frameworks to improve charge storage and pulse power performance in sediment microbial fuel cells. The P. orientalis wood was first carbonized, functionalized with cobalt- and nickel metal-organic frameworks formed using benzene-1,3,5-tricarboxylic acid as the organic ligand, and then subjected to a second pyrolysis step to obtain self-supported composite cathodes. Structural and surface characteristics were examined using Fourier transform infrared spectroscopy, Field-emission scanning electron microscopy, Brunauer-Emmett-Teller surface area analysis, Raman spectroscopy, and X-ray diffraction. Electrochemical performance was evaluated using electrochemical impedance spectroscopy and galvanostatic discharge tests. The nickel-functionalized and cobalt-functionalized cathodes showed surface areas of 346.4 and 327 m2 g−1, respectively. Compared with the unmodified carbonized wood cathode, the MOF-functionalized cathodes exhibited lower impedance, smaller initial voltage drops, lower equivalent series resistance, faster voltage recovery, and higher apparent capacitance. The highest apparent capacitance reached 151.7 mF at −1.5 mA and a 5 s pulse duration for the nickel-functionalized cathode. In addition, the modified cathodes delivered a maximum pulse power density of about 3 W m−2. These results showed that cobalt- and nickel metal-organic framework functionalization improved the electrochemical response of carbonized wood cathodes and provided a sustainable route to developing high-performance cathodes for sediment microbial fuel cells.