Rapid urbanization along with intensive solar radiation increases the surface temperature of buildings. The heated surfaces further lead to growth in the ambient temperature and subsequently lead to urban heat island. This leads to a higher demand for electricity, mostly in the summer, which in turn has an adverse effect on global warming. It is potentially feasible to utilize the thermal energy from the sunlight to alleviate these problems. The thermoelectric phenomenon is a viable option to convert available thermal energy to electricity for power generation in buildings. Cement, common building material, and their composites are attractive for making low-priced thermoelectric materials to convert trapped thermal energy in the building surfaces into electricity. However, the realization of this potential is limited yet due to the low thermoelectric conversion efficiency of cement composites. Improving conversion efficiency via composite engineering and incorporating thermoelectric cement at the building surfaces may generate electricity, which can be possibly achieved for powering small-scale devices. This chapter reveals a way to improve the thermoelectric properties of cement composites with the addition of graphene nanoplatelets. The different weight percentages of graphene are blended with cement and then compressed to fabricate bulk composites. On bulk samples, the thermoelectric properties are measured.