Silk fibroin (SF) is a promising and versatile biodegradable protein for biomedical applications. This study aimed to develop a prolonged release device by incorporating SF microparticles containing dyes into SF hydrogels. The influence of dyes on incorporation and release kinetics in SF based devices were evaluated regarding their hydrophilicity, molar mass, and cationic/anionic character. Hydrophobic and cationic dyes presented high encapsulation efficiency, probably related to electrostatic and hydrophobic interactions with SF. The addition of SF microparticles in SF hydrogels was an effective method to prolong the release, increasing the release time by 10-fold.