The combination of the steel-FRP composite bar (SFCB) and engineered cementitious composite (ECC) holds favorable applications in terms of durable resilient structures. However, a clear understanding of the interfacial bond performance of this novel combination is currently lacking. Therefore, the bond behavior and mechanism of the SFCB-ECC interface were investigated through direct pullout tests. A total of 48 cube specimens were fabricated, with the test variables including bar type, bar diameter, embedment length, and matrix type. The experimental results indicated that the bond failure mode of SFCBs and FRP bars differed from that of deformed steel bars, attributed to the damage of resin-rich ribs in relatively high-strength ECC. The bond-slip curves revealed both the fundamental differences and similarities among steel bars, SFCBs, and FRP bars. The Poisson effect and shear lag effect increased with a decrease in bar stiffness and an increase in diameter. The combined impact of the interaction between the bar stiffness and diameter resulted in varying bond strengths for steel bars, SFCBs, and GFRP bars, despite their similar surface geometries. A theoretical model for the bond strength at the SFCB-ECC interface was derived using the thick-walled cylinder principle and subsequently validated with test data. Finally, a unified empirical model framework for predicting the bond strength of various bar-matrix combinations was proposed based on the theoretical model. The accuracy of this method was evaluated using a collected database.