Provided in various embodiments are surface-modified hydrogels and hydrogel microparticles, methods for their preparation, and uses thereof for delivery of personal care and healthcare active ingredients, and agricultural active ingredients. In some embodiments, such hydrogels and hydrogel microparticles comprise surface coatings that are resistant to solvent washing and can act as barriers for the migration of water and/or water-compatible alcohols and actives soluble therein.