The eutectoid Ti–Cu alloy has the advantages of high strength and hardness. However, the pearlite eutectoid structures with coupled α + Ti2Cu lamellae result in low plasticity. In this study, a Zr alloying method is proposed to suppress the formation of lamellar pearlite and promote a bainite-like morphology. Increasing the Zr content can transform the α lamellae into rod-like laths and the Ti2Cu lamellae into dispersed particles, thereby reducing their embrittlement effect. The α laths are further refined to about 0.27 and 0.37 μm with 30% and 50% Zr addition, resulting in strong grain boundary strengthening effects. As a result, the mechanical properties are enhanced after Zr alloying. The best combination of compressive yield strength, maximum strength, and plasticity is achieved with 30% Zr addition, which is about 1040 MPa, 2505 MPa, and 33%, respectively. The results in this study can offer valuable insights into microstructure optimization and performance enhancement in active eutectoid Ti–Cu systems.