When it is asked, “where can refractory metals be used?,” the possible shortest answer is, “where cannot they be used?” The uses of refractory-metal-based compounds in research and industry are too many to be enumerated; nevertheless, some outstanding examples are briefly mentioned here. Essentially, chalcogenide forms of refractory metals are preferred in the fabrication of high-performance structures. Therefore, expanding the current studies that usually focus on tungsten- and molybdenum-based structures to other materials may open new opportunities. Moreover, research on ternary and quaternary structures can also be a keystone in creating high-performance products. The rationale of the present review is to give a brief overview of the recent history of refractory-metal-based chalcogenides (RMCs). Initially, the framework is confined to the general design and approaches for the synthesis of refractory metal chalcogenides. The assay is continued by extending with characteristic features of materials from crystalline properties to thermoelectric attributes and examining device fabrication processes. Taken together, the device fabrication part where RMCs are mainly used is extensively focused upon. Finally, outlook and future perspectives are given on the design and construction of RMCs to enable future inspiration and innovation.