Multilayer structures of graphene oxide‐zinc oxide nanorods (GO‐ZnONRs) hybrids are successfully grown for use as an active material in resistive switching random access memory (RRAM) devices. A considerable reduction in the OFF current is achieved through a layer‐by‐layer growth of GO‐ZnONR multilayers up to three repeating layers as the active material. The scanning electron microscope images and X‐ray diffraction patterns of the hybrid multilayer structures reveal that vertically oriented ZnONRs are sandwiched between GO sheets. A Raman analysis shows that the G peak position in GO redshifts, due to the COZn bonding at interfaces of the hybrid multilayer structures. X‐ray photoelectron spectroscopy analysis of the hybrid multilayer structures also confirms the growth of GO on ZnONRs and secondary ZnONRs on GO, through a COZn bonding. This study realizes the growth of vertically oriented secondary and tertiary ZnONRs on GO, accompanying a tuning of photoluminescent emission wavelength. This hybrid multilayer structure‐based resistive memory device exhibits a stable resistive switching behavior with an ON–OFF ratio up to 3.3 × 105, which is higher by three orders of magnitude than the ON–OFF ratio of a single‐layer ZnONRs based device.

Hollow nanostructures exhibit a wide range of potential applications because of the quantum confinement effect that arises from the narrow width of such nanostructures. It is challenging to synthesize hollow nanostructures of 2D materials. A facile top‐down approach is presented for synthesizing high‐quality hollow graphene nanostructures from highly oriented pyrolytic graphite target. Hollow graphene nanostructures composed of few‐layered graphene nanorings (GNRs) are synthesized in acetone and poly(4‐vinylpyridine) (P4VP) using the laser ablation in liquid technique. Density functional theory calculations of the layered GNRs indicate that their bandgap converges with an increase in the number of layers. To demonstrate the feasibility of the synthesized NRs for use in device applications, flexible two‐terminal devices with a Pt/GNRs‐P4VP/indium tin oxide structure are fabricated; the devices exhibit excellent memory characteristics, with the ON/OFF ratio being 2 × 104 and the retention time being 105 s. These results suggest that synthesizing uniform bandgap‐engineered GNRs in organic media through laser ablation is an excellent method for realizing high‐density, low‐cost nonvolatile memories in a scalable manner.