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Collagen, one of the most popular biomedical materials, exhibits rapid biodegradation accompanied by a notable decrease of mechanical stability in the human body. This is a key challenge for its use in large-sized tissue regeneration, which takes a long time. In order to resolve this problem, we introduced vapor-phase titanium (Ti) derivatives into the interchain regions in collagen via TiO2 atomic layer deposition (ALD), which has been widely used for thin-film deposition. The introduced Ti simultaneously enhanced both the tensile strength (∼384.45 MPa) and Young’s modulus (∼1.56 GPa) by approximately 29 and 26% compared to the pristine commercial collagen membrane. In vitro tests demonstrated that approximately 31% of Ti-infiltrated collagen is retained after 4 weeks, whereas the pristine commercial collagen rapidly degrades by up to 90% within 1 week. The in vivo biodegradation rate was greatly improved and inversely proportional to the number of TiO2 ALD cycles. Moreover, bone mineralization, which is observed during the late stage of bone healing, appeared only in the Ti-infiltrated collagen. We believe that our simple vapor-phase treatment method could be widely used with xenograft materials, which typically require adequate biodegradation rates and stable mechanical properties.