in certain improper ferroelectrics. [3] This is important for the electronic polarizability that plays an important role in this class of materials, and underlies the hyperferroelectric behavior, specifically the resistance to depolarizing field. The key condition is the instability of longitudinal optic modes in addition to active transverse optic instability characteristic of normal ferroelectrics. This provides a mechanism for canceling the depolarizing field. As shown in Figure 1, a number of these hyperferroelectrics adopt a polar stuffed wurtzite structure which is typically formed by an ABC stoichiometry (A, B, and C represent different elements). [4] This mechanism motivates us to extend the range of materials by searching for a different class of covalent-polar compounds, ABC 2 , exemplified by LiAlTe 2 . [5] It provides opportunities for designing switchable devices since it is compatible with substrates such as germanium tellurium (GeTe), which are prototypical phase change memory materials.The ABC 2 ternary compound β-LiAlTe 2 has a layered polar covalent tetrahedral structure, space group, P3m1 (156). [5a] As shown in Figure 1a, this quadruple-layered (QL) crystal is formed by an in-plane covalent bonded AlTe 4 tetrahedral layer with Li atoms located in the distorted trigonal antiprisms, with van der Waals (vdW) bonding between the QL. This vdW bonding suggests that in addition to being polar, such material may be an amenable formation in single QL form as a 2D material. This raises the possibility of having a hyperferroelectric 2D layered material based on the phase with an out-of-plane polarization. In most case, there are two major approaches to obtain polarization in 2D materials: (a) functionalization of nonpolar 2D materials; (b) searching for 2D intrinsic ferroelectric materials. [6] The former strategy uses chemical doping or surface passivation to produce switchable dipoles. [7] The latter approach is to find materials with intrinsic 2D polarization, such as Janus 2D materials. [8] These derivative 2D materials with broken mirror symmetry attracted considerable attention because of their unique properties, such as large piezoelectric effect, Rashba spin splitting, and second-harmonic generation response.