“…Ferroelectric materials have received intensive attention in the past decades due to their potential applications in electronic devices such as nonvolatile memory. − The growing demand of ultrahigh density storage requires a smaller size for functional domains as well as ultrathin thickness. ,− However, the traditional ferroelectric oxides on the nanoscale have been limited by the long-standing issue of critical thickness, below which the ferroelectric polarization would disappear. ,, The recently discovered two-dimensional (2D) ferroelectric materials shine a light on the development of ultra-high-density memory as the nanoscale 2D ferroelectrics can retain a sizable polarization with extraodingary electronic properties. − With the inherent stable, layered structure and clean surface, 2D van der Waals (vdW) materials are suitable candidates to study ferroelectricity at the limitation of the atomic layer. ,− Among the various 2D ferroelectric vdW materials demonstrated in experiments, ,,− the 2D vdW material In 2 Se 3 was reported to maintain spontaneous polarization even at monolayer thickness. ,,, The monolayer In 2 Se 3 has quintuple atomic layers in the sequence of Se–In–Se–In–Se, and the spontaneous polarization originates from the atomic displacement of the middle Se layer. The unique atomic structure leads to an intrinsic coupling of the in-plane (IP) and out-of-plane (OOP) polarizations, , resulting in multifunctional applications such as electromechanical transducer and artificial intelligence synapse devices. ,, The excellent optical and ferroelectric properties of In 2 Se 3 also make it promising for applications in optoelectronics, photovoltaics, and information processing. ,,, Given its wide applications, great efforts have been devoted to achieve the synthesis of large-scale 2D In 2 Se 3 with a uniform thickness.…”