A mode-locked laser operating at a frequency over 10 THz is reported, which is three orders of magnitude greater than a standard mode-locked laser. The system used molecules with a Raman gain as an amplifier, while coherent molecular motions were used for optical modulation. Molecules in a high-finesse optical cavity modulated a continuous-wave beam to produce a train of ultrashort optical pulses at a repetition rate corresponding to the frequency of molecular motion. Phase-locking was achieved by an appropriate compensation of the total dispersion of the optical cavity. Thus, the oscillating multiple longitudinal modes were all coupled under phase-matching conditions of parametric four-wave mixing.