We experimentally observed a possibly enhanced self-phase modulation (SPM) in silicon suspended membrane waveguides (SMWs) by measuring the spectral broadening of optical pulses. The nonlinear coefficient n2 and the two-photon absorption coefficient β2 of silicon SMWs were measured to be (4.6 ± 0.9) × 10−18 m2 W−1 and 0.46 cm GW−1 at 1555 nm wavelength. We also proposed a method of using SPM-induced spectral broadening to obtain the coupling loss of a single grating coupler and experimentally compared the spectra of two grating couplers in silicon SMWs and in silicon-on-insulator waveguides.