Porous silicon layers on wafers are commonly converted into particles by mechanical milling or ultrasonic fragmentation. The former technique can rapidly generate large batches of microparticles. The latter technique is commonly used for making nanoparticles but processing times are very long and yields, where reported, are often very low. With both processing techniques, the porosity and surface area of the particles generated are often assumed to be similar to those of the parent film. We demonstrate that this is rarely the case, using air-dried high porosity and supercritically dried aerocrystals as examples. We show that whereas ball milling can more quickly generate much higher yields of particles, it is much more damaging to the nanostructures than ultrasonic fragmentation. The latter technique is particularly promising for silicon aerocrystals since processing times are reduced whilst yields are simultaneously raised with ultrahigh porosity structures. Not only that, but very high surface areas (> 500 m2/g) can be completely preserved with ultrasonic fragmentation.