Transition metal dichalcogenides (TMDs, chemical formula MX2, M = transition metal, X = S, Se, Te) are a class of two-dimensional materials consisting of individual MX2 layers stacked by van der Waals forces. Among them, molybdenum disulfide (MoS2) has been studied extensively in a wide range of fields such as electrochemical energy storage, electrocatalysis, electrochemical water desalination, or tribology . As a consequence, a large number of synthesis approaches resulting in diverse morphologies and/or crystallite sizes are reported in literature. While exfoliation or gas phase deposition methods like chemical vapor-or atomic layer deposition can produce mono-/few-layered materials with high precision, hydrothermal methods can be employed to obtain MoS2 with varying morphology in larger quantities. For the latter, morphology, particle/crystallite size, or crystallinity can be tuned by variation of synthesis parameters. Specifically, it was demonstrated that lowering the pH of the reactant solution of the hydrothermal synthesis will yield smaller crystallite sizes. Other studies have shown that the lattice parameters of MoS2 can be directly tuned, for example, by the introduction of foreign species / pillars into the interlayer space, expanding the c-lattice parameter. This includes top-down approaches like the topotactic insertion of alkylammonium cationic pillars as demonstrated by Schöllhorn et al., however a previous chemical reduction and ion exchange are required. In summary, the structural properties of MoS2 can be tuned individually by different approaches at several length scales, from macroscopic tuning of particle or crystallite size, down to the microscopic tuning of lattice parameters like the interlayer spacing. It would be desirable to control MoS2 structure over several length scales at once in a one-pot synthesis approach, allowing to readily tailor emerging MoS2 functional properties.