Poly(L-lactic acid) (PLLA) is of interest in drug delivery applications for its biodegradable and biocompatible properties. Polymer-controlled drug delivery relies on the release of embedded drug molecules from the polymer matrix during its degradation. PLLA degradation exhibits an induction period, during which an insignificant amount of degraded products and embedded drug can be released. Due to this induction period, drug release is initially nonlinear, a complication in drug delivery applications. PLLA degradation is a function of crystallinity, such that control over its crystallinity tailors drug release over time. In this study, the effect of laser-induced PLLA crystallinity reduction on degradation is investigated. Samples having lower surface crystallinity are shown to have higher rates of molecular weight reduction and earlier mass loss than nonlaser-treated samples, as observed from gel permeation chromatography and mass change. Wide-angle X-ray diffraction measurements show that crystallinity increases with degradation. A numerical model is implemented from hydrolysis and diffusion mechanisms to investigate the effect of laser irradiation on biodegradation. Controlled laser treatment of PLLA offers a method for constant drug release through the reduction of surface crystallinity.