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Bio-waste derived nanocelluloses show excellent mechanical flexibility and self-aggregated capability, which enable them to be good supporting substrates for the synthesis of electroactive materials. Herein, we present a facile route for fabricating composite aerogels consisting of carbonized nanocellulose fibers (CNF) and mixed-valent manganese oxide (MnOx), toward supercapacitor applications. Mixed solutions of nanocellulose and manganese acetate with different ratios were prepared and freeze-dried into hybrid aerogels. The hybrid aerogels were then transformed into CNF/MnOx composites by a calcination process. The CNF membranes served as porous carbon nano-reservoirs for MnOx and electrolyte. The CNF/MnOx composites also kept a 3D porous aerogel structure with hierarchical pores, which enabled stable transport of both electrolyte ions and electrons to the electrode surface, leading to low a charge-transfer impedance and good electrochemical kinetics. The CNF/MnOx-based symmetric supercapacitor showed a satisfied energy density and power density of 37.5 Wh kg−1 and 2.75 kW kg−1, respectively. All the above results demonstrate the feasibility of using sustainable nanocellulose as a nanoscale carbon substrate for the synthesis of hybrid composite electrodes toward renewable supercapacitor applications.