Degradable polymers are beginning to play an increasing role as materials for environmental and medical applications. Understanding factors that control erosion, such as bond cleavage and the dissolution and diffusion of degradation products, will be critical to the future development of these materials. Erosion kinetics, photomicroscopy, and infrared spectroscopy were used to understand the erosion mechanism of two families of degradable polymers, polyanhydrides and polyesters. Polyanhydrides exhibit behavior more characteristic of surface erosion, whereas the polyesters exhibit bulk erosion patterns. Control of erosion times from a few days to several years can be achieved by a judicious choice of monomer units and bond selection.