Designing of high-performance, low-cost, and nonprecious metal-based bifunctional electrocatalysts is highly significant for the development of water splitting process and expanding the practical application of green hydrogen production. Transition metal dichalcogenides (TMDs) with intrinsic physical and chemical properties have been considered potential catalytic materials for electrode fabrication. However, it has remained challenging to develop TMD catalysts that have bifunctional properties for overall water splitting. Herein, WSe2, as a typical representative of TMDs, was utilized to design electrocatalysts using polypyrrole (PPy) or polyaniline (PANI) as a conducting polymer (CP) and cobalt doping. A facile hydrothermal preparation of WSe2 in the presence of CP enabled the construction of cobalt-doped WSe2@CP electrocatalysts. Morphological analysis indicated that the CP played an important role as a conductive template to enhance the distribution of WSe2 nanosheets, leading to higher surface area. In addition, cobalt doping led to the formation of defect structures and boosted the electrocatalytic activities of the catalysts for oxygen evolution reaction (OER). Owing to the increased electrochemical surface area and defect structures, the cobalt-doped WSe2@CP nanostructures exhibited enhanced electrochemical properties for hydrogen evolution reaction (HER) and OER in an alkaline medium. The cobalt-doped WSe2@PANI modified glassy carbon electrode (GCE) exhibited overpotentials down to 308 and 360 mV at a current density of 10 mA cm−2 for the HER and OER, respectively. Furthermore, the cobalt-doped WSe2@CP electrocatalysts demonstrated long-term stability and continuous cycling. More importantly, the Co–WSe2@PANI electrolyzer required cell voltage of 1.87 V at a current density of 10 mA cm−2 for overall water splitting process. This work provides new findings for designing efficient bifunctional electrocatalysts utilizing TMD materials and conducting polymers.