Herein, we have isolated onion-like nanocarbon (ONC) from the exhaust soot of diesel engines and further doped it with nitrogen (N) and sulfur (S) to fabricate N,S-co-doped ONC (N-S-ONC). To explore its application feasibility, we have assembled an aqueous Zn-ion hybrid supercapacitor (ZIHSC) with a N-S-ONC cathode, which attains high specific capacitance with good rate capability. In-depth analyses suggest that the mechanism of charge storage in the ONC is governed by both capacitive-controlled and diffusion-controlled processes, with the capacitive processes leading at all sweep rates. The ZIHSC demonstrated a good energy density of 50 Wh/kg, a maximum power density of 3.6 kW/kg, and an impressive cycle life with 73% capacitance retention after 50,000 charge-discharge cycles. The study suggests the potential possibly for the long-term application of BC derived nanocarbon in electrochemical energy storage systems (EESSs).