In this report, for the first time, the non-modified glassy carbon electrode was used for detection of cardiovascular drug interaction with bovine serum albumin (BSA). These interactions were tested at physiological conditions (T = 37 °C and pH = 7.4 phosphate buffer solution) in different incubation times (0-4 h) by cyclic voltammetry (CV), differential pulse voltammetry (DPV) and square wave voltammetry (SWV). The applications of DPV for quantitative investigation of some cardiovascular drug interaction with BSA (as a model of serum albumin proteins) were discussed. The herein described approach is expected to promote the exploitation of electrochemically-based methods for the study of drug-serum albumin protein interaction which is necessary in biochemical and biosensing studies. This report may open a new window to application of electrochemical sensors towards interactions of cardiovascular drugs with BSA and human serum albumin (HAS) in the near future.