Ni-20Cr-Eu2O3 composites were designed as new control rod materials and were synthesized from Ni, Cr, and Eu2O3 mixture powders via ball milling and vacuum hot pressing. During ball milling, Eu2O3 was fined, nano-crystallized, amorphized, and then dissolved into matrix. The effect of Eu2O3 content on the microstructure and mechanics was researched, and the corresponding mechanism was discussed. The relative densities, grain sizes, and microhardness increased when Eu2O3 content increased. According to the TEM observations, Eu2O3 particles showed a semi-coherent relationship with the matrix. The results of mechanical property testing showed that the ultimate tensile strength, yield strength, and elongation decreased with the Eu2O3 content increased. The maximum ultimate tensile strength, yield strength, and elongation were 741 MPa, 662 MPa, and 4%, respectively, with a 5 wt.% Eu2O3 addition. The experimental strengths were well matched with the theoretical values calculated by the strengthening mechanisms indicating that this method was highly effective for predicting the mechanical properties of Ni-20Cr-Eu2O3 composites.