We report the first systematic observations of relativistic self-phase-modulation (RSPM) due to the interaction of a high intensity laser pulse with plasma. The plasma was produced in front of a solid target by the prepulse of a 100 TW laser beam. RSPM was observed by monitoring the spectrum of the harmonics generated by the intense laser pulse during the interaction. The multipeaked broadened spectral structure produced by RSPM was studied in plasmas with different density scale lengths for laser interactions at intensities up to 3.0 x 10(19) W cm(-2) (a=p(osc)/m(e)c=4.7). The results are compared with calculated spectra and agreement is obtained.