Ca alloying is beneficial for improving the uniform elongation for friction stir processed (FSPed) Mg-4Al-2Sn-xCa (0, 0.5, 1.0 and 1.5 wt.%) (AT42-xCa) alloys. Coarse CaMgSn and Al2Ca particles in as-cast AT42-xCa alloys lead to a sharp decrease in elongation. Friction stir processing (FSP) is effective in improving strength and elongation by refining grain structure along with CaMgSn and Al2Ca particles, and inducing grain orientations with high Schmid factors for basal slip. Consequently, FSPed AT42-0.5Ca alloy exhibits simultaneously enhanced ultimate tensile strength (∼224 MPa) and elongation (∼30.9%). Compared to the Ca-free alloy, 0.5 wt.% Ca alloying increases the heat input and promotes the dislocation recovery, reducing residual dislocations. Nano-sized CaMgSn precipitates in grain interiors inhibit the dynamic recovery of dislocations during tensile, facilitating the work-hardening ability. Besides, high Schmid factors facilitate basal dislocation slips. Therefore, high EL is primarily due to the dislocation-free fine grain (∼2.7 μm), refined CaMgSn particles (micron-sized particles (∼1.3 μm) and nano-sized precipitates (∼55 nm)) and high Schmid factors (∼0.446) for basal slips.