Targeting amyloid-β (Aβ)-induced complex neurotoxicity has received considerable attention in the therapeutic and preventive treatment of Alzheimer's disease (AD). The complex pathogenesis of AD suggests that it requires comprehensive treatment, and drugs with multiple functions against AD are more desirable. Herein, AuNPs@POMD-pep (AuNPs: gold nanoparticles, POMD: polyoxometalate with Wells-Dawson structure, pep: peptide) were designed as a novel multifunctional Aβ inhibitor. AuNPs@POMD-pep shows synergistic effects in inhibiting Aβ aggregation, dissociating Aβ fibrils and decreasing Aβ-mediated peroxidase activity and Aβ-induced cytotoxicity. By taking advantage of AuNPs as vehicles that can cross the blood-brain barrier (BBB), AuNPs@POMD-pep can cross the BBB and thus overcome the drawbacks of small-molecule anti-AD drugs. Thus, this work provides new insights into the design and synthesis of inorganic nanoparticles as multifunctional therapeutic agents for treatment of AD.