Transition metal chalcogenides have nowadays garnered burgeoning interest owing to their fascinating electronic and catalytic properties, thus possessing great implications for energy conversion and storage applications. In this regard, their controllable synthesis in a large scale at low cost has readily become a focus of research. Herein we report diatomite-template generic and scalable production of VS2 and other transition metal sulfides targeting emerging energy conversion and storage applications. The conformal growth of VS2 over diatomite template would endow them with defect-abundant features. Throughout detailed experimental investigation in combination with theoretical simulation, we reveal that the enriched active sites/sulfur vacancies of thus-derived VS2 architectures would pose positive impacts on the catalytic performance such in electrocatalytic hydrogen evolution reactions. We further show that the favorable electrical conductivity and highly exposed sites of VS2 hold promise for serving as sulfur host in the realm of Li−S batteries. Our work offers new insights into the templated and customized synthesis of defect-rich sulfides in a scalable fashion to benefit multifunctional energy applications.