Layered transition metal chalcogenides (MX, M = Mo, W, Sn, V; X = S, Se, Te) have large ion transport channels and high specific capacity, making them promising for large-sized Na + /K + energy-storage technologies. Nevertheless, slow reaction kinetics and huge volume expansion will induce an undesirable electrochemical performance. Numerous efforts have been devoted to designing MX anodes and enhancing their electrochemical performance. Based on the metal-organic assembly strategy, nanostructural engineering, combination with carbon materials, and component regulation can be easily realized, which effectively boost the performance of MX anodes. In this Review, we present a comprehensive overview on the synthesis of MX nanostructure using the metal-organic assembly strategy, which can realize the design of MX nanostructures, based on self-sacrificial templates, host@guest tailored templates, postmodified layer and derivative templates. The preparation routes and structure evolution are mainly discussed. Then, Mo-, W-, Sn-, V-based chalcogenides used for Na + /K + energy storage are reviewed, and the relationship between the structure and the electrochemical performance, as well as the energy storage mechanism are emphasized. In addition, existing challenges and future perspectives are also presented.