There is huge interest in biosensors as a result of the demand for personalized medicine. In biomolecular detection, transition-metal dichalcogenides (TMDs) can be used as signal-enhancing elements. Herein, we utilize a solution-based electrochemical exfoliation technique with bipolar electrodes to manufacture MoSe2 nanolabels for biomolecular detection. Prepared MoSe2 nanoparticles (NPs) exhibit electrocatalytic activity toward the hydrogen evolution reaction (HER), and such a property allows it to act as a robust label for magneto-immunoassays toward protein detection. The magneto-immunoassay also displayed good selectivity, a wide linear range of 2 to 500 ng mL-1, high sensitivity (LOD = 1.23 ng mL-1) and reproducibility (RSD = 9.7%). These findings establish the viability and reproducibility of such an exfoliation technique for TMD nanolabels for the development of low costs and efficient biosensing systems. (Graph Presented).