Provided herein are core-shell heterostructures design comprising a metal (e.g., noble metal) nanoparticle core and a transition metal dichalcogenide (TMD) shell, and methods of preparation and use thereof. In particular embodiments, the core-shell heterostructures described herein are synthesized by direct growth of a monolayer or multilayer fullerene-like TMD shell on a metal (e.g., noble metal) nanoparticle core, exhibit unique Raman scattering and photoluminescence characteristics, and are useful, for example, in plasmonic hot electron enhanced optics and optoelectronics.