We experimentally and theoretically investigated the second-harmonic (SH) radiation from spherical gold nanoparticles as function of the particle radius in the range from 40 to 100 nm. By fitting the measured SH intensity to an analytical model, we demonstrated size-dependent second-order susceptibility tensor components, which significantly increase by reducing the size of the particles. Finally, we found new SH polarization diagrams for large particle radii arising from the interference among the different multipolar terms.