With the advancement of ultra-fast and high-energy pulsed laser output, lasers have caused serious harm to precision instruments and human eyes. Therefore, the development of optical limiting materials with a fast response, low optical limiting threshold, and high damage threshold are important. In this work, for the first time, it is reported that phosphors Gd2O2S:Tb3+(GOS) displays exceptional functionality in laser protection. GOS with sizes of 11 μm, 1 μm, and 0.45 μm are prepared. Based on the optical limiting and Z-scan technology systems under 532 nm and 1064 nm nanosecond laser excitation, the nonlinear optical properties of GOS are investigated. It is found that GOS exhibits outstanding optical limiting properties. In addition, the optical limiting response of GOS is size-dependent. Concerning the largest particle size, GOS has the best nonlinear optical response, while the precursor shows no nonlinear optical performance. Meanwhile, GOS doped gel glass also displays excellent optical limiting properties with high transmittance, which preliminarily validates the application of GOS and other scintillators in nonlinear optics and encourages more research to better realize the potential of GOS.