We have studied magnetic and structural properties of ultrathin Ni films grown on PI(lII) surface using in situ surface magneto-optic Kerr effect and X-ray photoelectron spectroscopy. Perpendicular magnetic anisotropy was absent, and longitudinal Kerr signal was only detectable for Ni films thicker than 6 monolayers. Enhancement in longitudinal Kerr signal by 30% was achieved by post-annealing at temperatures below 800K, but upon annealing at 820K, surface alloy was formed. By using core-level binding-energy shifts, the composition was determined to be Ni 70 at. %.