and electronic properties compared to the bulk counterpart, which is subjected to the confinement of electrons in two dimensions in the former case. 2D nanosheets are a class of 2D nanomaterial consisting of sheet-like structures with lateral sizes ranging from a few nanometers to hundreds of micrometers [1] and widely being employed in electronic devices, [2][3][4][5] catalysis, [6][7][8] energy storage and conversion, [9,10] sensing, [11,12] and biomedicine. [13] In literature, numerous 2D nanostructures such as hexagonal boron nitride (h-BN), [14][15][16][17] transition metal dichalcogenides (TMDs), [1,[18][19][20][21] graphitic carbon nitride (g-C 3 N 4 ), [22,23] layered metal oxides, [24,25] layered double hydroxides (LDHs), [25,26] black phosphorus (BP), [27,28] silicene [29][30][31] and antimonene [32][33][34] have been engineered and subsequently, being utilized for various applications including catalysis, optoelectronics, energy storage/ conversion applications, etc.The 2D nanostructures are mainly categorized into "nonlayered" and "layered" crystal structures. So far, the exploration of 2D nanostructures has been restricted to naturally layered materials, that is, van der Waals (vdW) solids with strong in-plane chemical bonds but weak out-of-plane vdW bonds. These 2D layered materials are comprehensively investigated due to the single or few-layer nanosheet, which can be synthesized either by a top-down approach such as mechanical exfoliation, liquid exfoliation, etc., or a bottom-up approach such as chemical vapor deposition (CVD), wet chemical synthesis, etc. In definition, the naturally layered materials such as TMDs, MXenes, BP, etc. can be easily exfoliated or grown as atomically thin nanosheets due to the strong inplane chemical bonds but weak out-of-plane vdW bonds. [35,36] However, in recent years 2D nanomaterials on nonlayered crystal structures have been reported, such as ZnO, RuO 2 , IrO 2, etc. [35,37] Due to the inherent isotropic chemical bonds in three dimensions, the synthesis of 2D morphology is not as facile as the case of vdW solids, which requires stabilization of crystal structures far from thermodynamic equilibrium. Also, the typical thickness of these nonlayered 2D materials can be of a few layers of unit cells (0.5 nm to >10 nm) due to the absence of an intrinsic layered configuration. Therefore, 2D nanosheets of nonlayered materials Zinc oxide (ZnO) is a thermally stable n-type semiconducting material. ZnO 2D nanosheets have mainly gained substantial attention due to their unique properties, such as direct bandgap and strong excitonic binding energy at room temperature. These are widely utilized in piezotronics, energy storage, photodetectors, light-emitting diodes, solar cells, gas sensors, and photocatalysis. Notably, the chemical properties and performances of ZnO nanosheets largely depend on the nano-structuring that can be regulated and controlled through modulating synthetic strategies. Two synthetic approaches, top-down and bottom-up, are mainly employed for preparing Z...