Exploring cathode materials that combine excellent cycling stability and high energy density poses a challenge to aqueous Zn-ion hybrid supercapacitors (ZHSCs). Herein, polyaniline (PANI) coated boron-carbon-nitrogen (BCN) nanoarray on carbon cloth surface is prepared as advanced cathode materials via simple high-temperature calcination and electrochemical deposition methods. Because of the excellent specific capacity and conductivity of PANI, the CC@BCN@PANI core-shell nanoarrays cathode shows an excellent ion storage capability. Moreover, the 3D nanoarray structure can provide enough space for the volume expansion and contraction of PANI in the charging/discharging cycles, which effectively avoids the collapse of the microstructure and greatly improves the electrochemical stability of PANI. Therefore, the CC@BCN@PANI-based ZHSCs exhibit superior electrochemical performances showing a specific capacity of 145.8 mAh/g, a high energy density of 116.78 Wh/kg, an excellent power density of 12 kW/kg, and a capacity retention rate of 86.2% after 8000 charge/discharge cycles at a current density of 2 A/g. In addition, the flexible ZHSCs (FZHSCs) also show a capacity retention rate of 87.7% at the current density of 2 A/g after 450 cycles.