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In this study, we prepare Cr-doped Sb 70 Se 30 (SS) thin films via the magnetron sputtering. The influence of Cr doping on the crystallization behavior and structure characteristics of the SS thin films is systematically studied using a combination of experimental analyzes and theoretical calculations. The results reveal that compared with SS thin films, Cr-doped SS thin films exhibit higher crystallization temperature, better data retention capability, larger crystallization activation energy, and reduced resistance drift coefficient. In addition, the incorporation of Cr effectively suppresses grain growth in the SS thin films and refines the grain size. The electrical transport properties of the Cr-doped SS thin films are analyzed using a Hall system. Both X-ray photoelectron spectroscopy and first-principles calculations indicate that Cr is more prone to occupy Sb atoms and form stronger Cr–Se bonds, consequently enhancing the stability of the SS thin films. Raman spectroscopy confirms that the introduction of Cr leads to a decrease in bond length and an increase in bond energy. Moreover, the Cr-doped SS thin film exhibits minimal volume fluctuations and a smoother surface morphology, resulting in enhanced interface performance and reliability. Taken together, these results indicate that the introduction of Cr is an effective strategy for optimizing the properties and modifying the structures of SS phase-change materials. [ABSTRACT FROM AUTHOR]