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This article provides the first single-crystal XRD-based structure of enantiopure (R)-baclofen (form C), C10H12ClNO2, without any co-crystallized substances. In the enantiopure title compound, the molecules arrange themselves in an orthorhombic crystal structure (space group P212121). In the crystal, strong hydrogen bonds and C—H...Cl bonds interconnect the zwitterionic molecules.