Tertiary Amine Pendants‐Mediated Charge Regulation for Tunable Resistive Switching in Fully Printed NDI ‐ MXene Memristors

ABSTRACT Flexible in‐memory computing devices and neuromorphic computing systems urgently demand resistive random‐access memory devices that are compatible with large‐area, low‐cost printing technologies and feature tunable resistive switching behavior. Herein, an n‐type conjugated polyelectrolyte based on naphthalene diimide (NDI) acceptor skeleton is employed as an interfacial modifier, enabling the construction of a MXene@PNDIT‐F 3 N hybrid resistive switching layer. By integrating inkjet printing for the resistive layer deposition and screen printing for Ag electrodes, fully printed flexible memory devices with an effective area exceeding 20 cm 2 are successfully fabricated on fibrous substrates. The PNDIT‐F 3 N intercalates into the interlayer galleries of MXene and assembles uniformly on the nanosheet surfaces, introducing interfacial charge trapping/storage sites and strengthening interfacial charge coupling. The resultant devices exhibit reliable bipolar resistive switching behavior with a maximum ON/OFF ratio of 4.0 at an optimal PNDIT‐F 3 N mass fraction of 9.1%. These results demonstrate that side‐chain engineering‐mediated interfacial charge regulation enables the tailorable construction of capacitive‐resistive switching in MXene‐based resistive random‐access memory, laying critical material and processing foundations for fully printed flexible memristors.