High surface area materials can have a number of applications including use as pyrophoric devices, sensors, laser mirrors, filters, thermal barriers and catalysts. The aim of this work was to deposit highly porous thin films capable of undergoing a spontaneous pyrophoric reaction and igniting a suitable substrate material. Magnetron sputtering was the chosen deposition technique as it enables reproducible deposition of coatings, with closely controlled, almost uniform, thickness and morphologies over extended surfaces. A number of magnetron magnetic configurations were investigated and deposition conditions were varied in order to control the surface area of the films and, thereby, optimise the pyrophoric behaviour. As a consequence, pyrophoric coatings were produced with ignition temperatures dependent on the deposition conditions and substrate material/topography. When deposited on combustible substrates, these coating/substrate systems formed simple pyrotechnic devices in a one-stage process. The main thermal signal emitted by these devices was dependent on the substrate material only.