Studies on intercalation or substitution of atoms into layered two-dimensional (2D) materials are rapidly expanding and gaining significant consideration due to their importance in electronics, catalysts, batteries, sensors, etc. In this manuscript, we report a straightforward method to create sulphur (S) deficient molybdenum (Mo) sulfide (MoS2−x) structures and substitute them with zerovalent copper (Cu) atoms using a colloidal synthesis method. The synthesized materials were studied using several techniques to understand the proportion and position of copper atoms and the effect of copper functionalization. Specifically, the impact of change in the ratio of Cu : S and the hydrogen evolution reaction (HER) activity of the derived materials were evaluated. This technique paves the way for the synthesis of various functionalized 2D materials with a significant impact on their physical and chemical behavior making them potential candidates for catalysis and several other applications such as energy storage and the development of numerous functional devices.