We have investigated the self-assembly of ultrathin zirconium coordination monomer and polymer films using a layer-by-layer approach. These materials are of great interest for incorporating metal ion (inorganic) moieties in organic (polymer) films with applications ranging from conductors to catalytic materials. The differences between the polymer and monomer assembly from solution are described. These differences were investigated using UV-vis spectroscopy, AFM, and surface plasmon spectroscopy. The differences in orientation, morphology, roughness, and linearity of deposition reflect the conformational limitations of the polymer toward self-assembly. On the other hand, the sequential assembly of the monomer and Zr metal ion indicates the strong coordination between the metal and the organic ligands, resulting in robust homogeneous films.