Previously, we have demonstrated how graphene can be simultaneously electrochemically exfoliated and functionalized , as well as combined with 1T-MoS2 , and here we extend this work to 2H-MoS2. In order to avoid either losing the desirable semiconducting properties of MoS2 or creating unwanted defects, we demonstrate a convenient and efficient way of functionalizing the 2H-MoS2 directly without any pretreatment. Briefly, thin functionalized MoS2 (fct-EEM) flakes of high quality can be obtained electrochemically through simultaneous exfoliation and functionalization using TBA + (tetrabutylammonium) in the electrolyte. In this simultaneous exfoliation and functionalization process, the MoS2 crystal was used as a cathode and graphite tape as the anode, therefore functionalized graphene can also be obtained at the same time as a byproduct. Un-functionalized pristine MoS2 and graphene were also fabricated as references to the functionalized materials. The functionalized MoS2 and functionalized graphene (fct-EEG) were characterised by Raman spectroscopy and XPS. We show that the functionalization for both 2H-MoS2 and the graphene was successful. The existence of the aryl diazonium salts not only functionalizes the MoS2, but also assists with the exfoliation process, leading to thinner MoS2 flakes. We then performed electrochemical measurements including cyclic voltammetry (CV), galvanostatic charge-discharge (GCD) and electrochemical impedance spectroscopy (EIS) on electrodes made of fct-EEM/fct-EEG composites to see how the functionalization can affect the electrochemical properties compared to unfunctionalized composite electrode. The functionalization increases the contribution of pseudocapacitance in the electrode, resulting in a higher specific capacitance. This promising technique, reported for the first time, opens up prospects in other applications such as sensing and HER, SERS (surface-enhanced Raman scattering) . The method can also be applied to functionalize other TMDs in order to enhance their properties to suit different applications.