We report the observation of spectral broadening induced by 200 femtosecond laser pulses with the repetition rate of 1 kHz at the wavelength of 532 nm in semi-insulating 4H-SiC single crystals. It is demonstrated that the full width at half maximum of output spectrum increases linearly with the light propagation length and the peak power density, reaching a maximum 870 cm −1 on a crystal of 19 mm long under an incident laser with a peak power density of 60.1 GW/cm 2 . Such spectral broadening can be well explained by the self-phase modulation model which correlates time-dependent phase change of pulses to intensity-dependent refractive index. The nonlinear refractive index n 2 is estimated to be 1.88×10 −15 cm 2 /W. The intensity-dependent refractive index is probably due to both the nonlinear optical polarizability of the bound electrons and the increase of free electrons induced by the two-photon absorption process. Super continuum spectra could arise as crystals are long enough to induce the self-focusing effect. The results show that SiC crystals may find applications in spectral broadening of high power lasers.