In this paper, we present the structural, mechanical and electrical properties of composite cement materials that can be widely used as substituent for cement. We start with the characterization of a composite cement sample using an analysis of X-ray diffraction (XRD) and nuclear magnetic resonance (NMR) spectra. The measurements of the Vickers hardness, cyclic and sweep linear voltammetry and electrochemical impedance spectroscopy (EIS) of composite cement materials were also recorded. This study compared the effect of the different nanocomposites added to cement on the mitigation of the alkali–silica reaction, which is responsible for the swelling, cracking and deleterious behavior of the material. The enhancement in Vickers hardness was more pronounced for composite cement materials. In contrast, the values of Vickers hardness decreased for the composite cement containing mortar and the control sample, suggesting that the long-term performance of cement was compromised. In order to obtain information about the bulk resistance of the composite cement material, electrochemical impedance spectroscopy (EIS) data were employed. The results suggest that for composite cement materials, there is an improvement in bulk electrical resistance, which can be attributed to the lower amounts of cracks and swelling due to lower expansion. In the control sample, a reduction in the bulk resistance suggests the formation of microcracks, which cause the aging and degradation of the material. The intersection of arcs in the EIS spectrum of the mixed composite cement sample gradually increased by an alkaline exposure of up to 21 days and finally shifted towards a low value of high frequency with an increase in alkaline exposure of up to 28 days.