Searching for efficient electrode materials with excellent electrochemical performance is of great significance to the development of magnesium-ion batteries (MIBs). Two-dimensional Ti-based materials are appealing for use in MIBs due to their high cycling capability. On the basis of density functional theory (DFT) calculations, we comprehensively investigate a novel two-dimensional Ti-based material, namely, TiClO monolayer, as a promising anode for MIBs. Monolayer TiClO can be exfoliated from its experimentally known bulk crystal with a moderate cleavage energy of 1.13 J/m2. It exhibits intrinsically metallic properties with good energetical, dynamical, mechanical, and thermal stabilities. Remarkably, TiClO monolayer possesses an ultra-high storage capacity (1079 mA h g−1), a low energy barrier (0.41–0.68 eV), and a suitable average open-circuit voltage (0.96 V). The lattice expansion for the TiClO monolayer is slight (<4.3%) during the Mg-ion intercalation. Moreover, bilayer and trilayer TiClO can considerably enhance the Mg binding strength and maintain the quasi-one-dimensional diffusion feature compared with monolayer TiClO. All these properties indicate that TiClO monolayers can be utilized as high-performance anodes for MIBs.