AbstractMagnesium (Mg) alloys with low concentrations of rare earth additions are known to exhibit strengths and ductility that are significantly higher than those obtained in traditional Mg alloys. However, the mechanisms that underlie these improvements are still open to debate. We assessed these mechanism(s) by carrying out in-depth analysis of the deformation behavior in single crystals of pure Mg and a homogenized Mg-0.75 at.% Gd alloy oriented for twinning, pyramidal- and basal-slip. We observed a fivefold increase in basal CRSS, an eightfold increase in twinning CRSS and a fourfold decrease of the pyramidal/basal CRSS (P/B) ratio due to Gd addition. We also observed that while twinning and pyramidal slip activities were similar in the two material systems, basal slip was radically different. Specifically, basal slip was planar in the alloy but wavy in pure Mg. Our work reveals that these observations are a consequence of Gd-rich short-range ordered (SRO) clusters in the alloy. We show that interactions between dislocations and the SRO clusters would lead to significant increases in strength and slip activity, and consequently, ductility improvements in homogenized polycrystalline Mg-Gd alloys.