Metal hydride hydrogen compressors have attracted great attention due to their reliable safety, environmental friendliness, and the absence of vibration and noise. Herein, the effects of Ti substitution for Zr on the crystal structure and hydrogen comprehensive performance of Ti0.92+xZr0.1-xCr1.0Mn0.6Fe0.4 (x = 0, 0.01, 0.02, 0.03) are investigated systematically. Among the investigated alloys, the Ti0.94Zr0.08Cr1.0Mn0.6Fe0.4 alloy can be considered as a promising candidate for application with a hydrogen capacity of 1.82 wt.% under 9 MPa at -10 °C. Meanwhile, it exhibits excellent hydrogen absorption kinetic performance, reaching 1.655 wt.% in 5 min. The desorption pressure at 83.9 °C is determined to be 25 MPa by Van't Hoff fitting plots, which fulfills the requirement of producing over 25 MPa hydrogen pressure in water-bath environments with a high compression ratio of 3.08. The Ti0.94Zr0.08Cr1.0Mn0.6Fe0.4 alloy is very promising for hydrogen refueling applications in long tube trailers and low-pressure gas cylinders.