In the present work, we performed the optimization of electrografting of adrenaline onto a glassy carbon electrode surface. The cyclic voltammetry technique was used to immobilize the compound on the electrode surface by immersing it in an acidic adrenaline solution. This grafting was achieved by conducting 20 successive CV scans over a wide potential range. The stability of the obtained layer was analyzed using the SWV technique. The conducted research shows that it is possible to create a stable adrenaline layer on the GCE surface using voltammetric techniques. Additionally, once a stable layer was immobilized, its sensitivity to certain metal cations—which cannot be directly detected electrochemically—was verified. After exposing the sensor to designated cationic solutions, there was a significant decrease in the adrenaline signal. This suggests potential future applications in cation determination.