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In this dissertation, a new and systematic material design approach is developed for ECC with added functions through material microstructures linkage to composite macroscopic behavior. The thesis research embodies theoretical development by building on previous ECC micromechanical models, and experimental investigations into three specific new versions of ECC with added functions aimed at addressing societal demands of our built infrastructure. Specifically, the theoretical study includes three important ECC modeling elements: Steady-state crack propagation analyses and simulation, predictive accuracy of the fiber bridging constitutive model, and development of the rate-dependent strain-hardening criteria. The first element establishes the steady-state cracking criterion as a fundamental requirement for multiple cracking behavior in brittle matrix composites. The second element improves the accuracy of crack-width prediction in ECC. The third element establishes the micromechanics basis for impact-resistant ECC design. Three new ECCs with added functions were developed and experimentally verified in this thesis research through the enhanced theoretical framework. A green ECC incorporating a large volume of industrial waste was demonstrated to possess reduced crack width and drying shrinkage. The self-healing ECC designed with tight crack width was demonstrated to recover transport and mechanical properties after microcrack damage when exposed to wet and dry cycles. The impact-resistant ECC was demonstrated to retain tensile ductility with increased strength under moderately high strain-rate loading. These new versions of ECC with added functions are expected to contribute greatly to enhancing the sustainability, durability, and safety of civil infrastructure built with ECC. This research establishes the effectiveness of micromechanics-based design and material ingredient tailoring for ECC with added new attributes but without losing its basic tensile ductile characteristics.