This paper presents a projectile impact analysis of high-performance fiber-reinforced cement composite (HPFRCC) structures based on the coupling of the finite element method (FEM) and the smoothed particle Galerkin (SPG) model in the LS-DYNA program. The K&C material model is calibrated for the HPFRCC. Through a quasi-static analysis using the calibrated model, the criteria for the element size of a FEM and the nodal particle distance of the SPG model are determined. Numerical simulations of the coupled SPG-FEM model are conducted to predict the structural responses of HPFRCC structures subjected to high impact velocities ranging from 342 m/s to 808 m/s. The results for the coupled model are compared with experimental data as well as numerical results for a pure FEM model to determine the relative accuracy and efficiency of a coupled FEM and SPG model for the large deformation problem. The convergence of the numerical results is also investigated in terms of the residual velocity and penetration depth. Moreover, the effects of various parameters on the models are discussed through a sensitivity analysis, and suitable parameter ranges that improve the accuracy of the numerical results are suggested.