The self-assembly of organic- inorganic compounds of palladium(II)-bis(N-long chain substituted imidazole) dichloride complexes has been investigated. The presence of a hydroxyl group at the 2-position of alkyl chain induced liquid crystal properties. Molecular ordering of Pd(II)imidazole complexes upon mechanical compression at the air/water interface is studied by surface pressure-area (pi-A) isotherms and Brewster angle microscope. Incorporation of lateral hydroxyl group in the alkyl chain enhances the stability of the films via intramolecular hydrogen bonding interactions. Langmuir-Blodgett (LB) films formed by these compounds were studied by various techniques to characterize their surface morphology, hydrophilic/hydrophobic property, surface functionalities and interlayer spacings. U-shaped interdigitated assembling, good crystallinity and in-air stability of these LB films were demonstrated. (c) 2007 Elsevier B.V. All rights reserved.