A general strategy for high performance nonvolatile polymer memory devices, with wrinkled reduced graphene oxide (rGO) films as electrodes and common insulating polymers as active layers, is proposed. The fabricated device exhibits electrical bistability and nonvolatile write‐once‐read‐many times‐type memory, with a low switching voltage of 2.7 V, high ON/OFF ratio of 104 and desirable long retention time over 104 s. The resistive switching of the device might be attributed to carbon‐rich filaments induced by the wrinkled rGO surface. Moreover, this polymer memory device based on a wrinkled rGO electrode can be further applied to flexible data storage systems. The strategy combining such advances in polymer memory devices with simple structure, common materials, excellent reproducibility, and high performance will demonstrate great potential in permanent archival storage applications.

and low energy operations in response to external or internal stimuli. [7,8] Stimuliresponsive resistive switching (RS) in twoterminal devices comprising of inorganic oxides, organic molecules, polymers, carbon nanomaterials, and their composites have emerged as attractive candidates for future memory materials. [9][10][11][12][13][14] Among these systems, polymer memories are especially promising, owing to their tunable structures, tailorable properties, facile engineering, and solution-phased fabrication processes. [15][16][17][18][19] Despite the great progress made in polymer memories for data storage and artificial synapse, [20][21][22][23][24] most of these systems could only perform single function. Therefore, it is not possible to fulfill several simultaneous requirements for practical memories, such as multimode function, varying speed, multilevel storage, and low power consumption.It has been previously shown, both experimentally and theoretically, that the memory performance of a polymer diode depends particularly on its active composition, device structure, interfacial design, and external stimuli. [25][26][27][28][29][30] Several strategies, including mechanism synergy, charge trap modulation, multilayer stacking, interfacial nanostructure, component blending, and suppressed stimuli, have been employed to boost and diversify the memory function of a single cell, resulting in multilevel storage, rectifying memory, low energy operation, and volatile and nonvolatile hybrid materials based memory. [31][32][33][34][35][36][37] However, to establish Emerging memory devices, that can provide programmable information recording with tunable resistive switching under external stimuli, hold great potential for applications in data storage, logic circuits, and artificial synapses. Realization of multifunctional manipulation within individual memory devices is particularly important in the More-than-Moore era, yet remains a challenge. Here, both rewritable and nonerasable memory are demonstrated in a single stimuli-responsive polymer diode, based on a nanohole-nanowrinkle bi-interfacial structure. Such synergic nanostructure is constructed from interfacing a nanowrinkled bottom graphene electrode and top polymer matrix with nanoholes; and it can be easily prepared by spin coating, which is a low-cost and high-yield production method. Furthermore, the resulting device, with ternary and low-power operation under varied external stimuli, can enable both reversible and irreversible biomimetic pressure recognition memories using a device-to-system framework. This work offers both a general guideline to fabricate multifunctional memory devices via interfacial nanostructure engineering and a smart information storage basis for future artificial intelligence.

Multilayer conjugated polymer nanofilms with desirable patterns and thicknesses were prepared by combining direct photopolymerization and in situ growth. Their optimized devices exhibited high performance nonvolatile memory effect.

Large-area patterned 2D conjugated microporous polymers (2D CMPs) were directly grown on SiO2/Si or reduced graphene oxide (rGO) surfaces with controllable film thickness and shape.