Memristive devices and systems have emerged as powerful technologies to fuel neuromorphic chips. However, the traditional two-terminal memristor still suffers from nonideal device characteristics, raising challenges for its further application in versatile biomimetic emulation for neuromorphic computing owing to insufficient control of filament forming for filamentary-type cells and a transport barrier for interfacial switching cells. Here, we propose three-terminal memristors with a top-gate field-effect geometry by employing a ferroelectric material, poly(vinylidene fluoride–trifluoroethylene), as the dielectric layer. This approach can finely modulate ion transport and contact barrier at the switching interface in non-filamentary perovskite memristors, thus, creating two distinct operation modes (volatile and nonvolatile). Additionally, perovskite memristors show desirable resistive switching performance, including forming-free operation, high yield of 88.9%, cycle-to-cycle variation of 7.8%, and low operating current of sub-100 nA. The dual-mode memristor is capable of emulating biological nociception in both active (perceiving pain) and blocked states (suppressing pain signaling).