Two-dimensional transition metal chalcogenides (2D-TMDs) have attracted much attention because of their unique layered structure and physical properties for transistor applications. Mechanically transferred metal contacts on these low-dimensional materials or their homogeneous and heterogeneous multilayers have generated huge interest to avoid deposition damages. In this paper, we show that there are large physical gaps at both the edge contact and surface contact between the transferred electrodes and the 2D materials. A method called laser shock induced superplastic deformation (LSISD) is proposed to tackle this issue and enhance the performance of the transistors. The enhancement mechanism was investigated by molecular dynamics (MD) simulations of the nanoforming process, atomic force microscopy (AFM), scanning electron microscopy (SEM), transmission electron microscopy (TEM) characterizations of the interfaces, and density functional theory (DFT) modeling. The force effect of laser shock can reduce the contact gap between metals and semiconductors. The electrical performances of the transistors before and after LSISD, along with MD simulations, are used to find the optimal process parameters. In addition, this paper applies the LSISD method to the short-channel MoS₂/graphene vertical transistors to show potential improvement in interface contact and electrical properties. This paper demonstrates the first report on using mechanical force induced by laser shock to enhance metal–semiconductor interfaces and transistor performances.