In this study, two different compositions of submicron-structured titanium (760 nm) and micron-structured chromium (4.66 μm) powders were mixed to fabricate Cr-31.2 mass% Ti alloys by vacuum hot-press sintering. The research imposed various hot-press sintering pressures (20, 35 and 50 MPa), while the sintering temperature maintained at 1250°C for 1 h. The experimental results showed that the optimum parameters of the hot-press sintered Cr-31.2 mass% Ti alloys were 1250°C at 50 MPa for 1 h. Also, the relative density reached 99.94%, the closed porosity decreased to 0.04% and the hardness and transverse rupture strength (TRS) values increased to 81.90 HRA and 448.53 MPa, respectively. Moreover, the electrical conductivity is enhanced to 1.58 × 104 S·cm–1. However, the grain growth generated during the high-temperature and high-pressure of the hot-press sintering process resulted in the grain coarsening phenomenon of the Cr-31.2 mass% Ti alloys after 1250°C hot-press sintering at 50 MPa for 1 h. In addition, the Cr-31.2 mass% Ti alloys were fabricated with the submicron-structured titanium (760 nm) and chromium (588 nm) powders showed more effective compaction than the micron-structured titanium (760 nm) and chromium (4.66 μm) powders did. The closed porosity decreases to 0.02% and the hardness values increase to 83.23 HRA. However, the agglomeration phenomenon of the Cr phase and brittleness of the TiCr2 Laves phases easily led to a slight decrease in TRS (400.54 MPa).