Acoustic vibrations of single gold nanorods coated with silver were investigated. We used single-particle pump–probe spectroscopy to monitor the silver deposition through the particle vibrations. Two vibration modes, the breathing mode and extensional mode, are observed, and the vibrational frequencies are measured as functions of the amount of silver deposited on single gold nanorods. The breathing mode frequency was found to decrease with silver deposition, while the extensional mode frequency was almost constant for silver shells up to 6 nm. The frequency changes agree with a model based on continuum mechanics and on the assumption of a uniform silver coating. The quality factors for the breathing mode and the extensional mode are hardly affected by silver deposition, indicating that the introduced interface between gold and silver contributes negligibly to the damping of the particle vibrations. Finally, we demonstrated that an atomic layer of silver can be detected using the particle acoustic vibrations.