Calcium silicate composite (CaO)(SiO) has significant applications in the bioactive materials in medical treatment and cementitious materials in construction engineering. In this study, to unravel the role of calcium atoms on the silicate composite, the molecular dynamics (MD) technique was used to simulate the structures, dynamics, and mechanical properties of (CaO)(SiO) systems, with x varying from 0 to 0.6. The Feuston-Garofalini model was employed to describe the interatomic interactions in the systems. Q species, the connectivity factor, shows that the increase in calcium content in the silicate composite can lead to the depolymerization of the silicate network. Due to the high diffusion rate, the presence of Ca atoms also weakens the stability of the chemical bonds in the system. With the increasing calcium content, the molecular structure of the silicate skeleton is transformed from an integrity network to separated short chains, which significantly decreases the stiffness and cohesive force of the calcium silicate composites. On the other hand, the uniaxial tension response of the calcium silicate composites suggests that at the postfailure stage, Ca atoms associate with the nonbridging oxygen atoms and the reconstructed Ca-O connection slows down the irreversible damage of the composite, hereby enhancing the plasticity.