A novel crumpled quaternary sulfur-doped nickel cobalt selenide nanoarchitecture grown on carbon cloth (S-(NiCo)Se/CC) has been successfully synthesized as an electrode material for high-performance ionic polymer-carbon cloth composite (IP-CCC) actuators. A facile one-step solvothermal process has been introduced here to synthesize S-(NiCo)Se/CC, resolving the time-consuming, complicated, and costly problems of existing methods. Taking advantage of the outstanding electron transport kinetics and three-dimensionally interconnected nature of the transition-metal chalcogenide structure, the hybrid carbon cloth electrode with quaternary sulfur-doped selenide nanoarchitectures exhibits low electrical resistivity (3 times lower than that of bare CC), high areal capacitance (409 mF/cm(2)), and excellent cycle stability (over 4000 cycles). Moreover, due to the synergistic effect between S-(NiCo)Se and a carbon cloth substrate, the S-(NiCo)Se/CC electrode-based actuator exhibits high blocking force (38.5 mN), 6 h durability, and large bending strain (0.47%). Compared with other actuators reported in the literature, the S-(NiCo)Se/CC electrode-based actuator shows much higher normalized blocking force, leading to opening of new potential applications in the field of next-generation soft electronics. Moreover, stacked multiple IP-CCC actuators in parallel exhibit an exceptional blocking force of 0.174 N under direct current 4 V.