The magnetic heterostructures provide flexible ways to realize particular magnetic properties that possess both scientific and practical significance. Here, by first-principles calculation, we predict strong Dzyaloshinskii–Moriya interactions (DMIs) by constructing CrI3/Metal heterostructures. The underlaying mechanisms are ascribed to the large spin-orbital coupling (SOC) of the I atom and the structural distortion in CrI3 layer caused by substrates. This is different from the traditional way that deposit magnetic films on substrate to generate DMI, wherein DMI is dominated by interlayer hybridization and large SOC of substrates. In addition, both Heisenberg exchange and magnetic anisotropy are modulated dramatically, such as Heisenberg exchange is nearly doubled on Au(111), and the out-of-plane magnetism is enhanced by 88% on Ir(111). Our work may provide a experimentally accessible strategy to induce DMI in layered magnetic materials, which will be helpful to the design of spintronics devices.