Sprayable high ductile fiber-reinforced cementitious composite (ECC), which exhibits tensile strain-hardening behavior in the hardened state, while maintaining sprayable properties in the fresh state, has been developed by employing parallel control of micromechanical design and rheological process design. Initially, micromechanical tools were adopted to properly select the matrix, fiber, and interface properties, and also to exhibit strain-hardening and multiple cracking behaviors in the ECC composites. Within the pre-determined micromechanical constraints, the fluid properties were controlled by the rheological process design to develop flocculations between cementitious particles at a proper rate. The sprayable properties of ECC mix were then developed by the controlled rheological properties of fresh matrix and the uniform dispersion of fibers. A series of spray tests showed the excellent pumpability, sprayability, and rebound property of tile sprayable ECC. Subsequent uniaxial tensile tests demonstrated that the mechanical performance of sprayed ECC is comparable to that of ECC cast with external consolidation, for the same mix design.