The development of inexpensive metal-free catalysts with high activity and stability as substitutes for carbon-supported platinum catalysts (Pt/C) in the oxygen reduction reaction (ORR) remains a great challenge. In this paper, we report a novel type of self-constructed, carbon nanoparticle (CNP)-coated porous biocarbon prepared from a natural, readily available, and renewable plant moss (Weisiopsis anomala) with a single precursor using template-free heat treatment. The CNPs were self-sponsored from the moss, which were simultaneously self-packed on the moss-derived carbon matrix via strong interactions between the hydroxyl and carbonyl functional groups of the CNPs and the moss-derived carbon matrix during the hydrothermal treatment. After being further carbonized at 900 degrees C, the moss-derived, CNP-coated biocarbon material had a larger surface area than that of the CNP-free, moss-derived biocarbon material. Electrochemical characterization showed that the CNP-coated biocarbon had a high activity in the ORR with an onset potential of 0.935 V vs. the reversible hydrogen electrode (RHE); this value is close to that of a commercial Pt/C catalyst (0.962 V vs. RHE) and is more positive than that of a CNP-free biocarbon material. The CNP-coated biocarbons also displayed a high limited current density, excellent long-term stability and resistance to methanol crossover, offering performance characteristics superior to those of Pt/C. Moreover, a microbial fuel cell (MFC) equipped with a CNP-coated biocarbon cathode outperformed an MFC with a Pt/C cathode in terms of energy output. This study presents a new approach for the production of inexpensive nanostructured carbon materials that exhibit high performance in the ORR from a natural resource. (C) 2015 Elsevier B.V. All rights reserved.