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 similar to 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 nanofilaments. This leads to the formation of hybrid gels with tunable mechanical strength by simply changing the charge number of the POMs. The H3PW12O40 (noted as PW) clusters@peptide hybrid hydrogels show excellent adsorption performance of dyes. Moreover, the long-range aligned PW clusters within the co-assembled fiber bundles exhibit great improvement in the efficiency of photodegradation of dyes, which shows 8.7 times higher than that of the pristine PW clusters in the homogeneous phase. The synergistic effect between the adsorption and catalytic process within the hybrid gels is considered to be responsible for its highly catalytic activity. This work highlights a general pathway upon the well-defined organization of the various components into hybrid materials with superior properties using simple peptide liquid crystals as templates. (C) 2020 Elsevier Inc. All rights reserved.