Eco-friendly techniques based on inorganic-binding peptides have been applied to modify titanium (Ti) surfaces. A prerequisite for preventing peri-implant mucositis and peri-implantitis is the adhesion of gingival soft tissue via epithelium sealing onto titanium surfaces. In this regard, the development of a rapid, convenient method for functionalizing Ti surfaces for the enhancement of epithelial sealing around abutments remains a critical challenge. In our study, Ti surfaces were modified to reinforce epithelial sealing using chimeric peptides constructed by connecting LNA3G3P and minTBP-1 with either L1 or L2. LNA3G3P is derived from the LG3 domain of the alpha 3 chain in Ln-5, which is the ligand of integrin alpha 6 beta 4 in the initiation of hemidesmosome (HD) assembly. The connection with minTBP-1 allows LNA3G3P to functionalize Ti surfaces by improving the HD anchorage of oral epithelial cells on Ti surfaces. Additionally, the chimeric peptide with L2 was more effective than that with L1 in improving epithelial sealing, which was ascribed to the capacity of L2 to provide a greater range for chimeric peptides to express their activity. Thus, this work successfully used Ti modification with chimeric peptides to improve epithelial sealing on Ti surfaces with the potential to prevent peri-mucositis and periimplantitis.