Laser concrete scabbling is the process by which the surface layer of concrete may be removed through the use of a low power density laser beam. The main aim of this investigation was to establish relationships between laser interaction time and volume removal for a wide range of material compositions, including different w/b ratios, binder compositions (OPC/PFA), aggregate/binder ratios and coarse aggregate sizes. The results show that 25% replacement of ordinary Portland cement with pulverised fuel ash and/or a reduced water/binder ratio improves the efficiency of scabbling of cement pastes. Mortars and cement pastes were seen to scabble at a constant rate, whereas concretes experienced a peak rate, after which volume removal reduced dramatically. Basalt aggregate concrete was less susceptible to laser scabbling than limestone aggregate concrete. The effects of composition on the mechanisms which drive laser scabbling are discussed. It is suggested that pore pressure spalling governs behaviour in cement pastes, and thermal stress spalling is more dominant in mortar specimens. The driving force responsible for laser scabbling of concretes is developed within the mortar.