Whey protein-based microcapsules containing a model drug, theophylline, were prepared in organic phase, using glutaraldehyde-saturated toluene. In all cases, spherical microcapsules, ranging from <400 to 1000 μm in diameter, were obtained. Results indicated that core crystals were embedded throughout the wall matrix. In all cases, retention efficiency of theophylline was higher than 74% and was not affected by cross-linking conditions. Results of theophylline release in simulated intestinal and gastric fluids at 37°C indicated that the diffusion-governed core release was significantly affected by size of microcapsules, cross-linking conditions, and by type of dissolution medium. In all cases, core release in simulated intestinal fluid was faster than in simulated gastric fluid.