The working load on automotive components is continuously rising, and the mechanical performance requirements for component materials are rising along with the growth trend toward light weight and high dependability in automobiles. In this study, the response characteristics of 51CrV4 spring steel were taken to be its hardness, wear resistance, tensile strength, and impact toughness. Prior to tempering, cryogenic treatment was introduced. Through the Taguchi method and gray relational analysis, the ideal process parameters were discovered. The ideal process variables were the following: a cooling rate of 1 °C/min, a cryogenic temperature of −196 °C, a holding time of 24 h, and a cycle number of three. An analysis of variance revealed that the holding time had the greatest effect on the material properties, with an effect of 49.01%. The yield limit of 51CrV4 was increased by 14.95% and the tensile strength was increased by 15.39% with this group of processes, and the wear mass loss was reduced by 43.32%. The mechanical qualities had a thorough upgrade. Microscopic analysis revealed that cryogenic treatment resulted in refinement of the martensite structure and significant differences in orientation. Additionally, bainite precipitation occurred, exhibiting a fine needle-like distribution, which positively influenced impact toughness. Analysis of the impact fracture surface showed that cryogenic treatment led to an increase in dimple diameter and depth. Further analysis of the elements revealed that calcium (Ca) weakened the negative effect of sulfur (S) on 51CrV4 spring steel. The overall improvement in material properties provides guidance for practical production applications.