Magnetocrystalline anisotropy has many advantages over shape anisotropy regarding coercivity in permanent magnets, making it a promising approach to enhance the coercivity of AlNiCo magnets. In this work, AlNiCo magnets with NdFeB-nanocrystalline phase were prepared by spark plasma sintering (SPS), and the effect of the NdFeB phase on coercivity was uncovered. AlNiCo powder with a spinodal structure and NdFeB powder with a nanocrystalline structure, which exhibit shape anisotropy and magnetocrystalline anisotropy, respectively, were sintered by SPS. With the advantages of low-temperature densification achieved by the SPS process, the spinodal and nanocrystalline structures were mostly retained. The microstructure analysis indicated that the SPS-ed magnet primarily consisted of AlNiCo regions with a spinodal structure, NdFeB regions with a nanocrystalline structure, and a transition region approximately 1~7 µm wide between them. A significant effect of the magnetic anisotropy of the NdFeB phase on magnetization behavior was found. The hysteresis loop of the SPS-ed magnets became single-phase magnetization, in contrast with the double-phase magnetization observed in the simple mixed powder. As the magnetocrystalline anisotropy of the NdFeB phase possesses higher coercivity, the coercivity of the SPS-ed magnet increased from 1250 Oe (of the AlNiCo raw powder) to 2490 Oe. This work provides valuable information for the coercivity enhancement of AlNiCo magnets.