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Low-alloyed Mg–Li–Er alloys were developed in this study and a bimodal-grained structure was obtained by varying the trace Er content and extrusion temperature. The alloys displayed a good strength–ductility synergy, i.e., a tensile yield strength (TYS) of 270 MPa and an elongation (EL) of 19.1%. Microstructural characterization revealed that the formation of numerous submicron Mg₂₄Er₅ particles favored a high density of low-angle grain boundaries (LAGBs) inside the deformed grains and inhibited dynamic recrystallization (DRX). The resultant coarse unDRXed grains with a strong basal texture and considerable LAGBs, together with the fine DRXed grains, contributed to the high strength–ductility synergy.