Currently, some TiZr-based high-entropy alloys have difficulty balancing strength and plasticity because of the large amount of brittle precipitation. This limitation hinders their engineering application as structural materials for complex components. Laser-directed energy deposition (LDED) technology provides unique advantages in composition design through the mixed element method and rapid nonequilibrium solidification. Therefore, the primary elements of the TiZr-based high-entropy alloys in this study were adjusted, leading to the achievement of a nonequiatomic Ti39 Zr39 Nb11 Mo5.5 V5.5 alloy with high relative density via LDED. Furthermore, a single-phase solid solution was obtained without the precipitation of brittle phases. The alloy exhibits excellent plastic deformation capability, with a compressive strain exceeding 50%. At a strain rate of 50%, the compressive stress reaches 2 194 MPa. Solid solution strengthening contributes approximately 75% of the yield strength, which is crucial to the high strength of the alloy.