This study used a facile method to develop a novel silver/Graphenepolypyrrole (Ag/G-PPy)-modified electrode that can be used as an electrochemical sensor for levosimendan detection. The properties of the synthesized Ag/G-PPy-modified electrode were examined through field-emission scanning electron microscopy, x-ray diffraction, and transmission electron microscopy.The Ag/G-PPy-modified electrode exhibited satisfactory current signals toward levosimendan concentrations ranging from 0.21 to 6.88 μM and exhibited a low detection limit (0.12 μM). Accordingly, the proposed electrode can serve as a simple and inexpensive electrochemical sensor for levosimendan detection.