Recently, 2D electron gases have been observed in atomically thin semiconducting crystals, enabling the observation of rich physical phenomena at the quantum level within the ultimate thickness limit. However, the observation of 2D electron gases and subsequent quantum Hall effect require exceptionally high crystalline quality, rendering mechanical exfoliation as the only method to produce high-quality 2D semiconductors of black phosphorus and indium selenide (InSe), which hinder large-scale device applications. Here, the controlled one-step synthesis of high-quality 2D InSe thin films via chemical vapor transport method is reported. The carrier Hall mobility of hexagonal boron nitride (hBN) encapsulated InSe flakes can be up to 5000 cm 2 V −1 s −1 at 1.5 K, enabling to observe the quantum Hall effect in a synthesized van der Waals semiconductor. The existence of the quantum Hall effect in directly synthesized 2D semiconductors indicates a high quality of the chemically synthesized 2D semiconductors, which hold promise in quantum devices and applications with high mobility.sufficiently large, i.e., ω c τ >> 1. However, the experimental magnetic field strength is typically limited, and the quantization condition subsequently requires long scattering time τ, or equivalently a high carrier mobility µ = eτ/m. Due to the high mobility requirement, the quantum Hall effect has only been observed in a handful of materials, most notably in epitaxially grown quantum wells. Apart from semimetal graphene, the quantum Hall effect recently has been observed in van der Waals (vdWs) semiconducting crystals which confine carriers within one to a few crystalline layers, e.g., 2D semiconductors of black phosphorus (BP) and InSe. [3][4][5] While the thickness of these vdWs semiconductors can technically be controlled within one layer, the production of such high-quality 2D semiconductors has been limited to mechanically exfoliated samples. As exfoliation produces crystalline flakes randomly, the geometry and thickness cannot be controlled well and it is the largest barrier toward the development of practical applications. Although great strides have been made in the synthesis of BP and InSe thin films using chemical vapor deposition (CVD) or other methods, [6][7][8][9][10][11] these 2D crystals' electronic properties are lacking compared to their exfoliated counterparts, due to their reactivity with ambient conditions. Thus far, the demonstration of the quantum Hall effect in a synthesized 2D semiconductor 2D Semiconductors