Flexible supercapacitors with excellent performance are needed to meet the increasing demand for wearable and flexible electronics. The challenge remains to design exceptionally flexible supercapacitors with remarkable electrochemical properties. Natural nacre shows outstanding fracture toughness due to its alternating inorganic and organic layered structure and abundant interfacial interactions, providing an inspiration for designing flexible supercapacitors. Herein, we demonstrated nacre-inspired flexible supercapacitors via synergistic interfacial interactions of π-π conjugated bonds, hydrogen bonding, and electrostatic interaction between halloysite (HA)-polyaniline (PANI) nanocomposites and graphene oxide (GO) nanosheets. The resultant nacre-inspired HPA-rGO nanocomposite films demonstrate strong tensile strength (351.9 MPa), high electrical conductivity (397.0 S cm−1), and long cycle life with ~ 85% of capacitance retention after 10,000 cycles. Furthermore, the assembled all-solid-state supercapacitors (ASSSs) based on bioinspired HPA-rGO electrodes can not only display extraordinary flexibility with no decay of capacitance behavior after 5000 bending cycles, but also deliver remarkable mass energy density up to 16.3 Wh kg−1, outperforming other flexible graphene-based supercapacitors. This nacre-inspired strategy for designing flexible electrodes provides an avenue for the next-generation power source in the fields of aerospace and smart wearable electronics.