C-2-symmetric nickel(II) salen complexes [NiL] 1 were deposited on a highly oriented pyrolytic graphite (HOPG) surface front their acetone solutions. They aggregate easily to single, segregated, homochiral polymeric chains of (M)-1D-(1)(n)[NiL] (2) on the substrate as also found in single crystals. In STM topography. the single helical 1D structures 2 found oil the surface were in excellent agreement with the dimension of aligned dimeric aggregates of 1 obtained from X-ray crystallography. Weak intermolecular (NiOMe)-O-II center dot center dot center dot coordinations (d(MeO-Ni) = 0.35 nm) were found to be responsible for the formation of the chiral, helical and 1D assemblies on the substrate.