This manuscript reports a new strategy to guide the chemical solution deposition of thin, microstructured metal films. The proposed strategy is based on the use of poly(2-(methacryloyloxy)ethyl ammonium chloride) (PMETAC) brushes grown via surface-initiated atom transfer radical polymerization as a template. Thin gold films have been prepared by first loading the PMETAC brushes with HAuCl4, followed by a NaBH4 mediated reduction to produce a PMETAC-gold nanoparticle composite film and finally an oxygen plasma treatment to remove the stabilizing polymer brush matrix and generate the desired thin gold film. The thickness of the gold films was found to scale with the thickness of the PMETAC brush template. This approach can also be extended to more complex, bimetallic films by exposing the PMETAC template successively to two different precursor salts. In this way, gradient type bimetallic palladium/gold films could be prepared.