Boron nitride nanosheet (BNNS) decorated with silver nanoparticles (AgNPs) was successfully synthesized via mussel-inspired chemistry of dopamine. Poly(dopamine)-functionalized BNNS (PDA-BNNS) was prepared by adding dopamine into the aqueous dispersion of hydroxylated BNNS (OH-BNNS) at alkaline condition. AgNPs were decorated on PDA-BNNS through spontaneous reduction of silver cations by catechol moieties of a PDA layer on BNNS, resulting in AgNP-BNNS with good dispersion stability. Incorporation of PDA on BNNS not only played a role as a surface functionalization method of BNNS, but also provided a molecular platform for creating very sophisticated two-dimensional (2D) BNNS-based hybrid nanomaterials such as metal nanoparticle-decorated BNNS.