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This paper reports on the development of high-performance fiber-reinforced cementitious composites (HPFRCC), taking into account environmental sustainability considerations. Engineered cementitious composites (ECC), a unique member of HPFRCC featuring high tensile ductility with ultra-high volumes of fly ash (HVFA) replacement (up to 85% by weight) of cement, are proposed in this paper. While micromechanics is applied in many aspects of the material design process, emphasis of this study is placed on the effect of fly ash content on altering material microstructure and mechanical properties. Experimental results show that HVFA ECCs, while incorporating high volumes of recycled fly ash, can retain a long-term tensile ductility of approximately 2 to 3%. Significantly, both the crack width and free drying shrinkage are reduced with an increase of the fly ash amount, which may benefit the long-term durability …