This paper demonstrates a new, reliable, and simple method for fabricating micropatterned nanoparticle arrays that can serve as templates for the surface-initiated polymerization of polymer brushes. As a proof of concept, we micropatterned gold nanoparticles (Au-NPs, approximate to 10 nm) onto glass, silicon, polystyrene, and gold surfaces by a simple three-step process: (1) microcontact printing of soluble polymer, (2) incubation with a solution of Au-NPs, and (3) lift-off of the template in a mixture of ethanol and deionized water. 40 pm wide features were successfully fabricated without any significant defects or nonspecific adsorption on the background. To demonstrate the utility of these Au-NP templates, we subsequently polymerized N-isopropylacrylamide by surface-initiated polymerization, using a surface-bound initiator.