Pulsed laser ablation is a simple, but versatile, experimental method that finds use as a means of patterning a very diverse range of materials, and in wide areas of thin film deposition and multi-layer research. Superficially, at least, the technique is conceptually simple also, but this apparent simplicity hides a wealth of fascinating, and still incompletely understood, chemical physics. This overview traces our current physico-chemical understanding of the evolution of material from target ablation through to the deposited film, addressing the initial laser–target interactions by which solid material enters the gas phase, the processing and propagation of material in the plume of ejected material, and the eventual accommodation of gas phase species onto the substrate that is to be coated. It is intended that this Review be of interest both to materials scientists interested in thin film growth, and to chemical physicists whose primary interest is with more fundamental aspects of the processes of pulsed laser ablation and deposition.