We present the preparation and characterization of novel metallosupramolecular thin films on solid substrates. These films incorporate metallosupramolecular polymers based on a tritopic cyclam bis-terpyridine ligand and are formed using different deposition techniques. From layer-by-layer (LBL) method, alternate thin multilayers of this metallosupramolecule along with oppositely charged polyelectrolyte are constructed by electrostatic self-assembly. Using dip-coating method, homogenous monolayers are deposited. The monolayer thickness is controlled by withdraw velocity of substrate. In a direct-assembly approach: Langmuir-Blodgett (LB), well-ordered metallosupramolecular monolayer is achieved by using a Metallosupramolecular Polyelectrolyte Amphiphile Complex (MPAC). The structures of these metallosupramolecular thin films are characterized by X-ray reflectivity (XRR), Atomic Force Microscopy (AFM), Langmuir isotherms, and UV/Vis absorption. The results open access to fabricate novel molecular materials such as sensors and memory devices. (C) 2013 Elsevier Inc. All rights reserved.