Chitosan is a nature-based polymer with low toxicity, excellent biocompatibility and biodegradability. However, the intractable solubility of chitosan in water and most conventional solvents hampers its biomedical applications. Following the dissolution method for dissolving chitosan in plain water developed by us, chitosan was dissolved in ionic liquid followed by overnight freezing at −20 °C and subsequent solvent exchange with plain water at room temperature. In this study, we fabricated a drug-carrying chitosan film via solution casting and air-drying by using the plain water-based chitosan solution. Specifically, brimonidine tartrate (BT), an antiglaucoma drug, was dissolved in the plain-water based solution and used to prepare BT-loaded chitosan film, i.e., chitosan-BT film. The resulting film is transparent, structurally stable, and mucoadhesive. Micro-sized antiglaucoma BT drug crystals form and are well dispersed in the chitosan film. The chitosan-BT film enables BT to have a high corneal permeability with fast drug release kinetics for potential ocular drug delivery.