In some embodiments, the present invention provides compositions including silk fibroin, at least one hydrophilic agent, and at least one catechol donating agent, wherein the at least one hydrophilic agent and at least one catechol donating agent are conjugated to the silk fibroin. According to various embodiments, at least a portion of the silk fibroin may be crosslinked. In some embodiments, the silk fibroin is at least 50% (e.g., 60%, 70%, 80%, 90%, 95% or more) crosslinked. In some embodiments, the present invention also provides methods for making such compositions.