Gold nanoparticles layered double hydroxide poly(vinyl alcohol) (Au NPs-LDH-PVA) hybrid films have been successfully prepared for the first time by bottom-up assembly of pretreated Au NPs-LDH nanosheets and subsequent spin-coating of PVA. The cross sections of the as-prepared hybrid films resemble the brick-and-mortar structure of nacre. The tensile strength of the Au NPs-LDH-PVA hybrid film reaches a high value of 122 MPa, which is higher than that of a pure PVA film and surpasses the strength of natural nacre. Furthermore, we demonstrate that Au NPs-LDH-PVA hybrid films possess surface-enhanced Raman scattering and catalytic properties. Therefore, our report on the fabrication of multifunctional Au NPs-LDH-PVA hybrid films not only shows a feasible route to functionalizing artificial nacre-inspired materials but also potentially broadens applications of these nacre-like materials.