Researchers have recently revealed that hybrid lead halide perovskites exhibit ferroelectricity, which is often associated with other physical characteristics, such as a large nonlinear optical response. In this work, the nonlinear optical properties of single crystal inorganic–organic hybrid perovskite CH3NH3PbBr3 are studied. By exciting the material with a 1044 nm laser, strong two-photon absorption-induced photoluminescence in the green spectral region is observed. Using the transmission open-aperture Z-scan technique, the values of the two-photon absorption coefficient are observed to be 8.5 cm GW−1, which is much higher than that of standard two-photon absorbing materials that are industrially used in nonlinear optical applications, such as lithium niobate (LiNbO3), LiTaO3, KTiOPO4, and KH2PO4. Such a strong two-photon absorption effect in CH3NH3PbBr3 can be used to modulate the spectral and spatial profiles of laser pulses, as well as to reduce noise, and can be used to strongly control the intensity of incident light. In this study, the superior optical limiting, pulse reshaping, and stabilization properties of CH3NH3PbBr3 are demonstrated, opening new applications for perovskites in nonlinear optics.