nearly 100%) with low-dimensional effect, thus having specific physical features that offer a wealth of potential to both scientific and industrial communities. [1][2][3][4][5] Extensive investigations have demonstrated that layered materials are the most common precursors to produce 2D nanostructures because these materials are constructed from stacked layers wherein weak van der Waals interactions hold together each interplane layer and strong chemical covalent bonding governs each individual in-plane layer. [5][6][7] Interestingly, 2D nanoplates can be readily prepared through two main well-established strategies, namely, the "top-down method" (mechanical cleavage, liquid-phase exfoliation, etc.) [1,[7][8][9][10][11] and the "bottom-up method" (e.g., chemical vapor deposition and wet-chemical methods). [12][13][14][15][16] Among these methods, liquid-phase exfoliation is considered to be quite promising and powerful due to its high output, large scalability, low cost, and simplicity. [7] Moreover, this method can produce nanosheets from most layered materials provided that the solvent's surface energy matches well with that of the target nanosheets. [7,17] The limited species and quantity, as well as the lack of certain properties, of 2D layered materials have motivated extensive investigations into 2D nonlayered materials, whose bulk counterparts are nonlayered and are held together strongly by chemical bonds in all three dimensions. [5,[18][19][20][21][22][23] In comparison with 2D layered materials, 2D nonlayered materials show distinct characteristics that their layered counterparts may not possess. Specifically, the surfaces of 2D nonlayered materials have abundant dangling bonds, which are absent on the surface of the layered materials, thereby offering numerous chemically active sites and resulting in improved catalytic capacity, [24][25][26] energy storage and conversion, [27,28] carrier properties, [18,29] etc. Due to these merits, considerable efforts have been made to fabricate 2D nonlayered materials. He and co-workers demonstrated a van der Waals epitaxial method to fabricate 2D nonlayered Pb 1−x Sn x Se nanoplates. [30,31] Zhang and co-workers synthesized nanosheets from the noble metal gold via a template-directed synthesis in which graphene oxide was developed as a 2D template for the growth of nonlayered materials. [32][33][34] Inspired by the concept of 2D layered materials, Sun and co-workers reported freestanding ZnSe single Investigations into 2D nanomaterials are of considerable significance from both an academic and industrial point of view. The present work addresses, for the first time, the fabrication of 2D nonlayered ultrathin selenium through a facile liquid-phase exfoliation method. The results reveal that the asprepared 2D Se nanosheets are 40-120 nm in lateral dimension and 3-6 nm in thickness. The nanosheets exhibit a trigonal crystalline phase similar to their bulk counterpart, indicating the conservation of the crystalline features during the exfoliation procedure. The success...