Zirconium hydride precipitation degrades the fracture toughness of nuclear reactor fuel cladding tube. Due to the difficulty of experiment, deep understanding on mechanical properties of zirconium hydride via numerical approaches is in a great need. To study the mechanical properties of zirconium hydride, the crystal plasticity finite element model considering geometrically necessary dislocations evolution is used to simulate the nanoindentation deformation behavior of single-crystal δ-hydride. The parameters in the crystal plasticity model are calibrated by Young's modulus along different crystallographic orientations and experimental stress-strain data at different strain rates. The predicted polycrystalline Young's modulus, Poisson's ratio, and nanoindentation hardness are in good agreement with the experimental results. The simulation results show that the nanoindentation hardness strongly depends on the indentation depth when it is smaller than 500 nm. Furthermore, the effects of crystallographic orientation and zirconium matrix on the indentation results are also studied. We find that the nanoindentation hardness of δ-hydride is slightly orientation dependent. For smaller hydride size or larger indentation depth, the surrounding zirconium matrix undergoes plastic deformation, which leads to a significant underestimate of the nanoindentation hardness of the hydride.