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These results could pave a potential wave for MIR photodetection and modulation with TMDC semimetals.Specific geometric morphology and improved crystalline properties are of great significance for the development of materials in micro-nano scale. However, for high-melting molybdenum (Mo), it is difficult to get high-quality structures exhibiting a single-crystalline nature and preconceived morphology simultaneously. In this paper, a pyramid-shaped single-crystalline Mo nanostructure was prepared through a thermal evaporation technique,