Several ruthenium(II) surfactants of general formula [Ru(bpy)₂L]²⁺ [L = N-(2-pyridylmethylene)-3,4-bis(tetradecyloxy)benzenamine, N-(2-pyridylmethylene)-3,4-bis(octadecyloxy)benzenamine, 9-(3,4-bis(tetradecyloxy)-benzenamino)-4,5-diazafluorene, 9-(4-(tetradecyloxy)-4′-azabenzenamino)-4,5-diazafluorene, 4,7-dinonadecyl-1,10-phenanthroline] and [Ru(L)₃]²⁺ (L = 4,7-dinonadecyl-1,10-phenanthroline) were synthesized and characterized by elemental analysis, ¹H NMR, UV-vis, luminescence spectroscopy, and cyclic voltammetry. Their Langmuir-Blodgett (LB) film formation properties and surface pressure-area (π-A) isotherms were also studied. Two complexes were found to show second-harmonic-generation (SHG) behavior.