Plasma-polymerized PMMA films were obtained by a low-temperature ambient deposition technique using a floating-electrode DBD jet with two distinct operation modes, namely a diffuse mode and a concentrated mode. Deposition rates, surface morphologies, atomic compositions, and chemical bond concentrations of the PMMA films showed a dependence on the modes. In the concentrated mode rapid deposition (22 nm · s-1) can be achieved with the substrate temperature merely rising to 39 °C. Besides transparent PMMA films with high quality, opaque films with wrinkled microstructures due to buckling effects were obtained. Similar functional groups to those in pure PMMA were also observed by both XPS and FTIR results. It was demonstrated that PMMA films can be successfully grown on different substrate materials, such as glass, plastic, rubber, onion skin, and fingernail. A PMMA film is deposited on a fingernail in ambient air by using a high-rate, low-temperature floating-electrode DBD jet. A transition from a diffuse mode to a concentrated mode and high deposition rates are observed with an increase in discharge powers. Transparent PMMA films as well as opaque films with wrinkled microstructures are obtained by adjusting the operation modes. © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.