A biomimetic approach is employed to deposit ceramic films on organic self-assembled monolayers (SAMs) coated substrates. Specifically, zirconia (ZrO2) films are grown in a zirconium sulfate precursor solution at near room temperatures (∼70°C). This process, directed by the nanoscale organic template, mimics the controlled nucleation and growth of the biominerals such as bones and teeth. The resultant zirconia films consist of nanosized particles (5-10 nm) that are precipitated out in a supersaturated precursor solution. Cross-sectional TEM and STEM works were performed to quantitatively analyze the film structure and chemistry, as well as interfacial region of the ceramic-SAM films. A stepwise deposition process was developed to avoid excessive formation of aggregation. Further, the dynamic nanoindentation testing was employed to assess the thickness and film-only intrinsic mechanical properties for direct comparison among the films processed with different processing parameters and microstructures. The films with finer particulate structure displayed higher intrinsic modulus than did those with coarser structure.