The rapid progress of smart and sustainable cities has led to an increased demand for construction materials that possess functional capabilities in energy storage and harvesting. In light of this, a comprehensive literature review is conducted in this study to investigate the multifunctional properties exhibited by carbon-based cementitious materials. Specifically, the piezoelectric, thermoelectric, tensile, compressive, and flexural behaviors of carbon fiber (CF), graphene, graphite powder (GP), and carbon nanotubes (CNTs) are thoroughly examined through multi-scale research approaches. The electrical conductivity and mechanical properties of these carbon-based additives are analyzed in relation to their molecular structures. Evaluation results reveal that CNTs-based cementitious composites demonstrate 160 %–269 % superior multifunctional performance compared to their CF-based counterparts. Furthermore, the feasibility of potential applications of carbon-based cementitious composites in concrete construction is extensively discussed, encompassing diverse areas such as thermoelectric energy harvesting, intelligent structural adjustment, cathodic protection systems, snow and ice melting, electromagnetic shielding, and structural health monitoring. The research outcomes presented in this study offer a systematic evaluation of a wide range of carbon-based cementitious materials, providing valuable guidelines and recommendations for engineers.