Molecular dynamic simulations have been performed to explore contact behavior, microstructure evolution and sintering mechanism of Al-Ni dissimilar nanoparticles under high-velocity impact. We confirmed that the simulated contact stress, contact radius, and contact force under low-velocity impact are in good agreement with the predicted results of the Hertz model. However, with increasing the impact velocity, the simulated results gradually deviate from the predicted results of the Hertz model due to the elastic-plastic transition and atomic discrete structure. The normalized contact radius versus strain exhibits a weak dependence on nanosphere diameter. Below a critical velocity, there are very few HCP atoms in the nanospheres after thermal equilibrium. There are two different sintering mechanisms: under low-velocity impact, the sintering process relies mainly on the dislocation slip of Al nanospheres, while the dislocation slip of Ni nanospheres and the atomic diffusion of Al nanospheres predominate under high-velocity impact.