Flexible bridge stay cables are often vulnerable to problematic vibrations under dynamic excitations. However, from an energy perspective, such excessive vibrations denote a green and sustainable energy source to some electronic devices (such as semi-active dampers or wireless sensors) installed on the same cables. This paper presents an experimental study on a novel dual-function system called electromagnetic damper cum energy harvester (EMDEH). The proposed EMDEH, consisting of an electromagnetic device connected to an energy-harvesting circuit (EHC), simultaneously harvests cable vibration energy and provides sufficient damping to the cables. A fixed-duty-cycle buck–boost converter is employed as the EHC, which emulates a resistive load and provides approximately optimal damping and optimal energy harvesting efficiency when operating in discontinuous conduction mode. A 5.85 m long scaled stay cable installed with a prototype EMDEH is tested in the laboratory under a series of harmonic and random excitations. The EMDEH can achieve a control performance comparable to passive viscous dampers. An average electrical power of 31.6 and 21.51 mW is harvested under harmonic and random vibrations, respectively, corresponding to the efficiency of 16.9% and 13.8%, respectively. Moreover, this experimental study proves that optimal damping and energy harvesting can be achieved simultaneously, which answers a pending question regarding such a dual-objective optimization problem. Self-powered semi-active control systems or wireless sensor networks may be developed for bridge stay cables in the future based on the proposed concept in this study.