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Twist angle between adjacent layers of two-dimensional (2D) layered materials provides an exotic degree of freedom to enable various fascinating phenomena, which opens a research direction—twistronics. To realize the practical applications of twistronics, it is of the utmost importance to control the interlayer twist angle on large scales. In this work, we report the precise control of interlayer twist angle in centimeter-scale stacked multilayer MoS2 homostructures via the combination of wafer-scale highly-oriented monolayer MoS2 growth techniques and a water-assisted transfer method. We confirm that the twist angle can continuously change the indirect bandgap of centimeter-scale stacked multilayer MoS2 homostructures, which is indicated by the photoluminescence peak shift. Furthermore, we demonstrate that the stack structure can affect the electrical properties of MoS2 homostructures, where 30° twist angle yields higher electron mobility. Our work provides a firm basis for the development of twistronics.