The optical Kerr effect of nanocomposites consisting of high refractive index (GaP) spheres is studied by means of three-dimensional finite-difference time-domain (FDTD) simulations at the wavelength of 532 nm. 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. The nonlinearity enhancement is more pronounced for the metasurfaces. Unexpectedly, the sign of the effective optical Kerr coefficient is inverted for some range of the sphere sizes above the Mie resonances.