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In the present study, we report the green and one-pot synthesis of silver nanoparticles (AgNPs) on as-prepared novel polyoxometalate {[Ni_2,5(Hpen)₄(PW₉O₃₄)] · 5H₂O} (POM) without any reducing agent and its application as improved anode material for lithium-ion batteries (LIBs). The structure of the AgNPs involved POM (AgNPs/POM) nanocomposite was characterized by transmission electron microscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. The synthesized POM was also characterized by elemental analysis and thermal analysis. The electrochemical performances of the POM, AgNPs, and AgNPs/POM composites were measured for charge/discharge specific capacities at different current rates in CR2032 coin-type cells. The prepared AgNPs/POM composite showed a high specific gravimetric capacity of about 1760 mAh g⁻¹ and long-term cycle stability.