The ever‐rising concerns with regards to energy shortages and climate change have made the search for clean and renewable energy sources a pressing priority for the sustainable development of societies. Although, conventional precious metal‐based catalysts such as platinum, iridium, and ruthenium are able to efficiently catalyze the conversion of chemical to electrical energy, they are often very costly, scarce, and suffer from poor stability, hence impeding their widespread applications. The limitations of the current state‐of art catalysts have propelled tremendous efforts in search for alternative catalysts. Notably, transition metal dichalcogenides (TMDs) have spurred much enthusiasm because of their natural abundance, low cost, and remarkable catalytic activity. Numerous studies have recounted that doping can tune the properties of TMDs and that vanadium dopants reportedly improve the electrical properties of Group 6 TMDs. Herein, the authors aspire to investigate the effects of doping varying amounts of vanadium on molybdenum dichalcogenides on their electrocatalytic activities toward hydrogen evolution reaction, oxygen evolution reaction, and oxygen reduction reaction. Despite previous studies bespeaking promising effects, the results here demonstrate both improvements and worsening of electrocatalytic performances from varying the stoichiometry of vanadium dopants in molybdenum dichalcogenides, depending on the type of materials and intended electrochemical applications.