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Highlights • Cu dendrites exclusively induced by Anderson type POM (NH 4) 4 [H 6 NiMo 6 O 24 ]. • Chemical association between POMs and Cu NPs was evidenced via XPS and Raman investigation. • Enhanced HER activity with NiMo 6 O 24 @Cu/TNA was achieved. • Mechanism of NiMo 6 O 24 @Cu/TNA electrochemical HER was investigated by Tafel study. • NiMo 6 O 24 @Cu/TNA system shows high stability with enhanced corrosion resistance under neutral and acidic environment. Abstract The design and synthesis of specific functional complex materials as desired catalysts for improved energy conversion and storage are of great importance and with grand challenges. Here, a facile synthesis strategy of Anderson POMs supported Cu dendrites toward electrochemical hydrogen evolution reaction with dramatically decreased overpotential under acidic aqueous condition is established in this work. We present the preparation of well crystallized Cu dendrites through co-electrodeposition on TiO 2 array with Anderson-type POM NiMo 6 O 24. Structural and state of valence investigation of the as-obtained electrocatalyst (NiMo 6 O 24 @Cu/TNA) evidence the specific morphology tunability and modification of Cu dendrites surfaces. During HER course, NiMo 6 O 24 can improve the H+ transfer and further help the H atom absorption which remedies the weakness of insufficient H atom absorption ability of Cu along with its strong electron transfer lowering overpotential upon HER. Therefore, HER with NiMo 6 O 24 @Cu/TNA is considerably enhanced by decreasing related overpotential of 130 mV compared to porous Cu foam. The modification of NiMo 6 O 24 endowed catalysts strong corrosion resistance assuring long term stability. Hence, the proposed strategy possesses improved activity and long term stability upon HER with NiMo 6 O 24 @Cu/TNA as electrocatalyst. Depending on the diversity of POMs, the current feasible and reliable heterogeneous electrocatalysts design with POMs would inspire more effective, low-cost strategies for energy conversion and open the pathway for large scale production. [ABSTRACT FROM AUTHOR]