The binary Ti-Zr congruent alloys have been a potential candidate for laser-directed energy deposition owing to an excellent combination of high structural stability and good formability. To solve its insufficient strength, a new series of Ti-Zr-Mo alloys with different Mo contents were designed based on a cluster model and then made by laser-directed energy deposition on a high-purity titanium substrate. The effect of Mo content on the microstructure and properties of the L-DEDed alloys was investigated. The consequences exhibit that the microstructure of all designed alloys is featured with near-equiaxed β grains without obvious texture. However, increasing Mo content induces a gradual refinement of the grain and a steady decrease in the lattice constant, which effectively improves the hardness, strength, wear and corrosion resistance of the designed alloys, but slightly weakens ductility and formability. From the viewpoint of both properties and forming quality, the Ti60.94Zr36.72Mo2.34 (at.%) alloy owns a proper match in mechanical, tribological, chemical, and forming properties, which is widely used in aeroengine components.