Second-harmonic generation (SHG) studies of C60 multilayer adsorbed on nickel crystal are presented. The experiments were performed in an ultra-high vacuum (UHV) chamber (10-10 mbar). The multilayer was prepared layer-by-layer making use of a Knudsen cell. The substrate was atomically prepared through heating cycles and ion bombardment. Low-energy electron diffraction (LEED) and Auger electron spectroscopy (AES) were used as tools for chemical and atomic structural analysis of the substrate. Second-harmonic generation of the nickel crystal (111) is also presented. The experiments were performed with the fundamental of a Nd-YAG laser, 1064 nm wavelength, 30 ps pulse width and 10 Hz repetition rate.