Magnesium oxide (MgO)-graphene oxide (GO) nanocomposites were prepared by the hydrothermal method at different temperatures. The effect of growth temperature on the structural, linear, and nonlinear optical (NLO) parameters was investigated. The decoration of MgO on GO sheets was confirmed by X-ray diffraction, scanning electron microscopy, Fourier transform infrared, and UV-visible (UV-vis) spectroscopy analyses. The energy band-gaps of MgO-GO nanocomposites were calculated from UV-vis spectrum using Tauc plot. The NLO parameters of MgO-GO nanocomposites were calculated for the first time by the simple Z-scan technique with nanosecond Nd:YAG laser at 532 nm. The nonlinear absorption coefficient β and nonlinear refractive index n 2 for MgO-GO nanocomposites at the laser intensity of 1.1 × 10 8 W/cm 2 were measured to be in the order of 10 −7 cm/W and 10 −12 cm 2 /W, respectively. The third-order NLO susceptibility of MgO-GO nanocomposites was measured in the order of 10 −9 esu. The results showed that MgO-GO structures have negative nonlinearity as well as good nonlinear two-photon absorption at 532 nm. Furthermore, the NLO parameters increased by the enhancement of the growth temperature. As the investigation of new materials plays an important role in the advancement of optoelectronics, MgO-GO nanocomposites possess potential applications in NLO devices.