As a potential next-generation battery technology, anode-free lithium metal batteries still face significant challenges in practical applications, primarily due to lithium dendrite growth, which leads to rapid capacity degradation and raises serious safety concerns. Unlike most strategies that engineer solid electrolyte interphases (SEI) through electrolyte additives or by directly applying artificial interphases, this study introduces an alternative approach by modifying the current collector to induce a more stable SEI in-situ. The surface-engineered bromine-functionalized one-dimensional titania lepidocrocite (Br-1DL) was synthesized by mixing 1DL with 4-bromocatechol, which binds to the surface through coordination with the two phenol groups. The Br-rich surface promotes the formation of a LiBr rich SEI with a lower lithium diffusion barrier during cycling, effectively suppressing dendrite growth and enhancing cycling stability. Utilizing the advantages of the 3D vertically aligned architecture, the 3D Br-1DL anode was evaluated through multiple electrochemical tests to examine its stability and performance in anode-free lithium metal batteries. The results show that Br-1DL exhibits lower overpotential and impedance and enables the symmetric battery to achieve a long cycling lifespan at high current density under room temperature conditions. This work proposes a potential pathway for enhancing the long-term stability of lithium anode-free batteries.