Ceramic films were deposited on polymer substrates from aqueous media at low temperatures through a bioinspired process. Specifically, zirconium oxide and titanium oxide films were deposited at 70°C on parylene substrates coated with phosphonate-terminated self-assembled monolayer (SAM). One purpose of this study is to deposit a strongly adherent ceramic protective layer on the polymer substrate. Adhesion of the ceramic films is evaluated by scratching the film over a 5-10 μm distance using a nanoindenter. An abrupt change in lateral force and friction coefficient while force is being ramped indicates the occurrence of delamination between the ceramic film and substrate. Accordingly, an adhesion testing protocol was developed to find such a critical normal force at which delamination of the films occurs. It was found that the films with a smaller clustered microstructure displays higher adhesion than those with a coarser counterpart. This experimental observation was further investigated by examining interaction energies between the in-situ formed ceramic nanoparticles and the SAM-coated polymer substrates in the aqueous deposition media based on the Derjaguin, Landau, Verwey, and Overbeek (DLVO) theory.