To improve room and elevated temperature mechanical properties of high-Nb TiAl alloys, Ti44Al6Nb1Cr alloy has been prepared by cold crucible directional solidification (CCDS) technique under loaded power of 40 kW and pulling rate of 8.3 μm/s. Macro/micro-structure and phase composition have been characterized. Tensile properties have been tested at room and elevated temperature and the related mechanisms have been revealed. Results show that equiaxed grains change to columnar grains growing up along the axial direction of ingot after CCDS. Phase component is still composed of α2, γ and B2 phases. Microstructure consists of lamellar clusters and network structure. The lamellar clusters in a grain possess the same orientation. The content and size of B2 phases decrease and some casting defects with small size decrease as well due to sufficient diffusion of Nb and Cr atoms under action of electromagnetic force during CCDS. Tensile results indicate that comprehensive mechanical properties of Ti44Al6Nb1Cr alloy are improved significantly after CCDS. At room temperature, ultimate tensile strength and total strain are 523 MPa and 3.03%, respectively, which are improved by 18.1% and 64.7% compared with that of as-cast Ti44Al6Nb1Cr alloy (443 MPa and 1.84%). Moreover, fracture morphology also indicates that there are many deep ravines between cleavage steps and some similar dimples microstructure on cleavage steps. They are beneficial to improving comprehensive mechanical properties. At 973 K, ultimate tensile strength of Ti44Al6Nb1Cr alloy does not decrease at all, still reaching 530 MPa after CCDS. When service temperature rises to 1173 K, the strain is less than 4.28% showing excellent mechanical stability under tensile stress less than 436 MPa. The excellent stability for mechanical properties is due to thin lamellar phases, directional microstructure and large plastic deformation region.