Cementitious materials having high damage tolerance and self-sensing ability are described herein. These materials may replace conventional concrete to serve as a major material component for infrastructure systems with greatly improved resistance to cracking, reinforcement corrosion, and other common deterioration mechanisms under service conditions, and prevents fracture failure under extreme events. These materials can also be used for the repair, retrofitting or rehabilitation of existing concrete structures or infrastructure systems. Furthermore, these materials may offer capacity for distributed and direct sensing of cracking, straining and deterioration with spatially continuous resolution wherever the material is located, without relying on installation of sensors. The present invention relates to multifunctional cementitious structural or infrastructure materials that integrate self-sensing with damage tolerance for improving safety, extending service life, and health monitoring of structures, components, and infrastructure systems.