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Natural polysaccharides are critical to a wide range of fields (e.g., medicine, food production, and cosmetics) for their various remarkable physical properties and biological activities. However, the bioactivities of naturally acquired polysaccharides may be unsatisfactory and limit their further applications. It is generally known that the chemical structure exhibited by polysaccharides lays the material basis for their biological activities. Accordingly, possible structural modifications should be conducted on polysaccharides for their enhancement. Recently, polysaccharides complexed with metal ions (e.g., Fe, Zn, Mg, Cr, and Pt) have been reported to be possibly used to improve their bioactivities. Moreover, since the properties exhibited by metal ions are normally conserved, polysaccharides may be endowed with new applications. In this review, the synthesis methods, characterization methods, and bioactivities of polysaccharide metal complexes are summarized specifically. Then, the application prospects and limitations of these complexes are analyzed and discussed.