“…Post-transition metal chalcogenides, including the two-dimensional gallium monochalcogenide (2D-GMC) family, have been becoming a rising star in the field of condensed matter physics and offering opportunities for engineering novel optoelectronic applications in recent years, thanks to possessing unique mechanical, electronic, and optical properties with the large optical window in 2D limit. In particular, noncentrosymmetric ε-phase gallium selenide (GaSe) that is commonly observed in various synthetic methods is one of the potential candidates for electronics, second-harmonic generation, especially for photoelectrochemical and photodetection applications with low dark current, relatively high photoresponsivity, and fast response time. − In addition, many researchers have demonstrated that leveraging hybrid dimensionality figure of merits, such as integration of 2D-layered materials with 3D substrates/templates via heteroepitaxy, could be a crucial benefit to enhance the performance of 2D-based optoelectronic devices. In fact, that allows for improving optical absorption efficiency, forming type-II band alignment mixed-dimensional heterostructures, and reducing unintentional contamination during chemical/mechanical exfoliation. ,− During the past decade, many efforts have been made to fabricate 2D/3D mixed-dimensional heterostructures by either chemical or physical deposition methods.…”