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In this work, we report a strategy to self-assemble multifunctional hydrogels composed of highly ordered polyoxometalates (POMs) helical arrays using a liquid crystalline tripeptide as the template. The cationic peptide can self-assemble into long-range ordered nanofilaments with a diameter of ~4.1 nm in aqueous media. Through the incorporation of various multivalent polyoxometalates (POMs), the POMs clusters can spontaneously organize into periodic nanowire arrays by the colloidal co-assembly with the as-prepared nematic peptide nanof