High‐index dielectric nanoantennas excited at Mie‐type resonances have exhibited enormous enhancement of optical nonlinearity. Such nanostructures have been actively studied by researchers in recent years. Here, a numerical analysis study of the optical Kerr effect of nanocomposites consisting of high refractive index (GaP) spheres at the wavelength of 532 nm is presented. This is done by means of 3D finite‐difference time‐domain simulations. The effective nonlinear refractive index of 0.8 µm thick nanocomposites and metasurfaces is evaluated. It is shown that the optical Kerr nonlinearity of the nanocomposites rises by orders in proximity to Mie resonances and may exceed the second‐order refractive index of the bulk material. It is revealed that the sign of the effective optical Kerr coefficient is inverted near the Mie resonances. This effect may be of interest in developing nonlinear optical metadevices.