The Boston keratoprosthesis (B-KPro) is globally the most commonly implanted artificial cornea for patients with severe corneal diseases, particularly those with multiple allograft failures. Despite providing a good visual recovery, the poor adhesion between the poly (methyl methacrylate) [PMMA]-made stem and the donor tissue poses a challenge, impacting the clinical outcome of the B-KPro. Using single-molecule covalent bonding, we herein functionalized PMMA surface with L-3,4-dihydroxyphenylalanine (L-DOPA) and studied its chemical, optical, mechanical, and biological properties. We have shown that the functionalization process alters the surface properties of the PMMA device and significantly improves its biocompatibility, without affecting the optical and mechanical properties of PMMA. Live/Dead assays showed that human corneal fibroblasts (HCF) seeded on L-DOPA surface have greater confluency (62.2 2.4%) compared to those of PMMA (19.1 1.8%) after 7 days of cell culture. In addition, HCF cultured on L-DOPA exhibited significantly higher metabolic rate (nearly twice) compared to those of PMMA, as indicated by AlamarBlue assay. Human corneal epithelial cells (HCEp) cultured on non-treated and treated PMMA also demonstrated a similar response. Moreover, immunocytochemistry revealed that HCF cultured on L-DOPA have a higher expression of ALDH3A1, Ki67, Integrin 1, and FAK with no expression of -SMA, compared to those of PMMA, which instead demonstrated greater expression of -SMA. These suggest that L-DOPA surface fosters cellular adhesion, proliferation, and migration, without adverse impact on the phenotype of the cells. This study offers an inexpensive and efficient tactic to covalently This article is protected by copyright. All rights reserved. modify the surface of materials such as PMMA with L-DOPA in order to achieve the optimal biocompatibility and biointegration of medical devices.