This paper studies the structure and mechanical properties of the Mg-1%Zn-xCa system subjected to high-pressure torsion (HPT) treatment. It was found that the chemical composition had a notable effect on the processes of grain refinement in the alloy. As is shown, HPT of Mg-1%Zn-0.005%Ca resulted in the formation of grains with a mean size of 250 nm, while HPT of the alloy with an increased content of Ca up to 0.2% led to the formation of a nanostructure with a mean grain size of 90 nm. It is demonstrated that high microhardness is typical of all HPT-processed samples. The formation of fine Mg2Ca particles was established to increase the heat resistance of the alloy.