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Reciprocating sliding friction tests were conducted on pure magnesium using a UMT-II tester. The tribo-chemical behavior was characterized using X-ray photoelectron spectroscopy (XPS) and electron probe micro-analyzer (EPMA), which showed that the tribo-chemical behavior of pure magnesium was due to a tribo-oxidation reaction. At room temperature, the debris layer on the worn surface contained Mg(OH)2, MgO, and MgCO3. According to the reciprocating sliding friction mechanism, the decomposition of MgCO3 into MgO should occur. XPS results revealed that the surface oxide layer, containing Mg(OH)2, and MgO, acted as a third layer to protect the surface. Apparently, Mg(OH)2·nH2O was the main tribo-chemical product of pure magnesium under sliding friction.