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[en] Highlights: • N,P,S-doped carbon nanofibers were prepared from affordable cellulose nanofibrils composites. • The obtained graphitic carbon could easily form 3D network with excellent mesopores and active sites. • High HER and ORR activities were manifested from the unique characteristics of carbon nanofibers. • Cellulose nanofibrils could be a promising platform for the development of effective carbocatalyst. Multi-element doped metal-free carbon nanomaterials with a 3D architecture were prepared from inexpensive and naturally abundant cellulose nanofibrils. Compared to the most graphene-based carbons reported in the literature that show only good oxygen reduction reaction (ORR) activity, our N,S-doped carbon nanofiber network coated with N,P-doped carbon nanoparticles showed good bifunctionality toward ORR and hydrogen evolution reaction (HER) activities. The HER performance with doped carbon material exhibited an onset potential of 233 mV (vs. RHE), a current density of 10 mA cm-2 at 331 mV (vs. RHE), and Tafel slope of 99 mV decade−1. The same material was also used for ORR, which could deliver an onset potential 10 mV more negative than commercial Pt/C and a cathodic peak of 0.84 V (vs. RHE). These values are better than most reported metal-free electrocatalysts. The superior performance of carbon hybrid may be attributed to the combination of a more exposed highly active N,P-doped carbon, a good integration of N,P-doped carbon with N,S-doped carbon nanofibers, and an accelerated electron transport through N,S-doped carbon nanofibers as good conductivity channels.