Mucus lines all surfaces of the human body not covered by skin and provides lubrication, hydration, and protection. The properties of mucus are influenced by changes in pH that may occur due to physiological conditions and pathological circumstances. Reinforcing the mucus barrier with biopolymers that can adhere to mucus in different conditions can be a useful strategy for protecting the underlying mucosae from damage. In this work, regenerated silk fibroin (silk) was chemically modified with phenyl boronic acid to form reversible covalent complexes with the 1,2- or 1,3-diols. The silk modified with boronic acid pendant groups has an increased affinity for mucins, whose carbohydrate component is rich in diols. These results offer new applications of silk in mucoadhesion, and the ability to bind diols to the silk lays the foundation for the development of silk-based sugar-sensing platforms.