Cascaded stimulated Raman scattering (SRS) of carbon disulfide (CS2) was investigated by a pulsed Nd:YAG laser with a wavelength of 532 nm. The fourth-order Stokes and second-order anti-Stokes lines were generated when the pump laser energy was about 1.909 mJ in one sample cell (C1) only. However, the same result was obtained in the second sample cell (C2) with a pump energy of 0.883 mJ. At the same time, the fifth-order Stokes line was produced in C2 when the pump energy increased to 1.208 mJ, and the coherent radiation wavelength ranged from 498 to 644 nm. The result was attributed to the resonance enhancement effect, where the frequency difference between the pump laser and the Stokes light emitted from the working medium (CS2) self-matched with the vibrational energy level of C=S, which resulted in the generation of the cascaded broadband SRS. The anti-Stokes SRS was attributed to four-wave mixing. Simultaneously, the pulse durations of the Stokes and anti-Stokes were compressed to about 380 ps by SRS and laser-induced breakdown. The resonance effect not only reduced the threshold, but it also generated broadband and short-pulse SRS.