Due to their potential improvement of high-temperature properties, the refractory metal hafnium (Hf) and the rare earth holmium (Ho) have attracted much attention. In the present research, NiAl-Cr(Mo) eutectic alloys with different Ho and Hf additions were fabricated by conventional smelting method and heat-treated to study the synergetic influence of strengthening elements and heat treatment. The samples were characterized using XRD, SEM, and TEM, and the three-point bending test was performed to obtain fracture toughness. The results demonstrate that Hf addition leads to the formation of Ni2AlHf Heusler phase and that Ho promoted the formation of Ni2Al3Ho phase. The microstructure of the alloy is affected by thermal treatment, with the coarsening of eutectic lamellae after heat treatment. The mechanical properties are improved by Hf and Ho additions, with increased fracture toughness. Overall, this study provides insights into the microstructure and properties of NiAl-Cr(Mo) eutectic alloys and highlights the potential of Hf and Ho addition to improve room-temperature properties. Specifically, the as-cast NiAl-Cr(Mo)-Hf eutectic alloy contains a relatively fine NiAl/Cr(Mo) eutectic lamella but coarse eutectic cell with Ni2AlHf phase embellished along the cell boundary. Minor Ho addition induces the formation of Ni2Al3Ho phase, which leads to the coarsening of the intercellular region but contributes to the refining of eutectic cell. In addition, the synergetic effect of Ho and Hf promotes the precipitation of Ni2Al3Ho and Ni2AlHf phases in the intercellular zone and increases the interface dislocations. Heat treatment benefits the solid solution of Ni2Al3Ho and Ni2AlHf phases, which improves their size and distribution by secondary precipitation. The Ni2AlHf phase in the NiAl-Cr(Mo)-Hf eutectic alloy becomes fine and uniformly distributed, but the NiAl/Cr(Mo) eutectic lamella in the eutectic cell becomes coarse. In comparison, heat treatment mainly optimizes the size and distribution of the Ni2Al3Ho and Ni2AlHf phases in the NiAl-Cr(Mo)-Hf-Ho eutectic alloy. Furthermore, heat treatment helps to eliminate the interface dislocations in the large NiAl precipitates and the NiAl/Cr(Mo) phase interfaces, which also contributes to fracture toughness by decreasing stress concentration. Minor Ho addition decreases the fracture toughness of as-cast NiAl-Cr(Mo)-Hf eutectic alloy from 6.7 to 6.1 MPa·m1/2, which should be ascribed to the coarsened intercellular region including aggregated Ni2Al3Ho and Ni2AlHf phases. However, minor Ho-doped NiAl-Cr(Mo)-Hf eutectic alloy obtained the highest fracture toughness of 8.2 MPa·m1/2after heat treatment. This improved fracture toughness should be mainly attributed to the refined and well-distributed Ni2Al3Ho and Ni2AlHf phases in the heat-treated NiAl-Cr(Mo)-Hf-Ho eutectic alloy.