In this paper, Sr was partially substituted by Li in the Zintl phase alloy SrAl2 and the structural and hydrogenation characteristics of the LixSr1-xAl2 (0 ≤ x ≤ 0.4) alloys were studied by X-ray diffraction (XRD), scanning electronic microscopy (SEM) and hydrogenation measurements. The alloy consists of a single Zintl phase of SrAl2 when x = 0. However, partial substitution of Sr by Li results in multiphase structure of the alloys. When x = 0.1 ~ 0.4, the alloys are all composed of SrAl2, SrAl4, Li2O and SrO phases. The content of Zintl phase SrAl2 in the alloy is decreased monotonously with the increase of x. Hydrogenation measurements were made at 473 K under 3 MPa hydrogen pressure. It is interesting to find that the initial activation and hydrogenation kinetics of the alloy are improved after small amount of Li substitution (x = 0.1 and 0.2), which could be attributed to the catalysis of Li2O phase.