Incorporating metal oxide nanoparticles into cement-based composites delays the hydration process and strength gain of cementitious composites. This study presents an approach toward improving the performance of bismuth oxide (Bi2O3) and gadolinium oxide (Gd2O3) particles in cementitious systems by synthesizing core–shell structures via a sol-gel process. Two types of silica coatings on cementitious pastes with 5% and 10% substitution levels were proposed. The rheology, hydration, and mechanical properties of the pastes were analyzed to determine the relationship between the coating type and nanoparticle concentration. The results indicate that despite the significant disparities in the performance of the resulting material, both methods are appropriate for cement technology applications. Bi2O3’s silica coatings accelerate the hydration process, leading to early strength development in the cement paste. However, due to the coarse particle size of Gd2O3, silica coatings exhibited negligible effects on the early age characteristics of cement pastes.