Experimental Ti-13%Zr and Ti-13%Zr-5%Cu alloys were made in an argon-arc melting furnace. The grade 2 CP Ti was used to control. The alloys were cast into phosphate bonded $SiO_2$ investment molds using an argon-arc casting machine, and The hardness and microstructures of the castings were investigated in order to reveal their possible use for new dental casting materials and to collect useful data for alloy design. The hardness of the Ti-13%Zr-5%Cu alloy(379Hv) became higher than that of Ti-13%Zr(317Hv) alloy, and the hardness of this alloys became higher than that of CP Ti(247Hv). Increasing in the hardness of the Ti-13%Zr-5%Cu alloy was considered to be solid solution hardening as the Ti-Zr system shows a completely solid solution for both high temperature $eta$phase and low temperature $alpha$ phase and also the inclusion of the eutectoid structure($alpha Ti+Ti_{2}Cu$). No martensitic structures are observed in the specimen made of CP Ti, but Ti-13%Zr and Ti-13%Zr-5%Cu alloys show a kind of martensitic structure. Ti-13%Zr-5%Cu shows the finest microstructure. From these results, it was concluded that new alloys for dental casting materials should be designed as Ti-Zr-Cu based alloys.