The incorporation of plasmonic metal nanostructures into semiconducting chalcogenides in the form of core−shell structures provides a promising approach to enhancing the performance of photodetectors. In this study, we combined Au nanoparticles with newly developed copper-based chalcogenides Cu 2 NiSnS 4 (Au/CNTS) to achieve an ultrahigh optoelectronic response in the visible regime. The high-quality Au/CNTS core− shell nanocrystals (NCs) were synthesized by developing a unique colloidal hot-injection method, which allowed for excellent control over sizes, shapes, and elemental compositions. The as-synthesized Au/CNTS hybrid core−shell NCs exhibited enhanced optical absorption, carrier extraction efficiency, and improved photosensing performance owing to the plasmonic-induced resonance energy transfer effect of the Au core. This effect led to a significant increase in the carrier density of the Au/CNTS NCs, resulting in a measured responsivity of 1.2 × 10 3 AW −1 , a specific detectivity of 6.2 × 10 11 Jones, and an external quantum efficiency of 3.8 × 10 5 % at an incident power density of 318.5 μW cm −2 . These results enlighten a new era in the development of plasmonic core−shell nanostructure-based visible photodetectors.