What musical notes can a molecule play? Carbyne is a chain of atoms that vibrates similar to an elastic string. Like the tuning of a guitar string, this vibration can be predicted based on length and tension. Using atomistic simulation, we determine the vibrational response of carbyne. We further produce audible notes, enabling specific musical composition with prescribed molecular conditions (pre-strain and length) and combine single chains into multi-chain systems to form molecular chords. Since the tension of a molecular chain is relatively low (<nN), such “strings” can potentially be developed for signaling and detection with high resolution.