In this work, we report a novel approach using proteinaceous microspheres of bovine serum albumin (BSA), human serum albumin (HSA) and silk fibroin (SF) containing different organic solvents, namely n-dodecane, mineral oil and vegetable oil, to reduce the activity of human neutrophil elastase (HNE) found in high levels on chronic wounds. The ability of these devices to inhibit HNE was evaluated using porcine pancreatic elastase (PPE) solution as a model of wound exudates. The results obtained indicated that the level of PPE activity can be tuned by changing the organic solvent present on different protein microspheres, thus showing an innovative way of controlling the elastase-antielastase imbalance found in chronic wounds. Furthermore, these proteinaceous microspheres were shown to be important carriers of elastase inhibitors causing no cytotoxicity in human skin fibroblasts in vitro, making them suitable for biomedical applications, such as chronic wounds.