Contrary to conventional ATRP, aqueous A(R)GET-ATRP at ambient temperature without deoxygenating reaction solutions is an extremely facile method to create polymer brushes. Using these techniques, extremely thick poly[2-(dimethylamino)ethyl methacrylate] polymer brushes can be prepared (∼700 nm), or reaction solutions can be low chemical-content, consisting of 99% v/v water. Based on these techniques, we have also developed an easy and inexpensive method, referred to as "paint on"-ATRP, that directly pastes reaction solutions onto various large-scale real-life substrates open to the air. The resulting brush surfaces possess excellent oil-repellent properties, which can be activated or deactivated in response to solution pH.