In this work, Fe2O3@TiO2 nanostructures with staggered band alignment were newly designed by an aerobic oil-phase cyclic magnetic adsorption method. XRD and TEM analyses were performed to verify the uniform deposition of Fe2O3 nanoparticles on the nanotube inner walls of TiO2. The steady-state degradation experiments exhibited that 1FeTi possessed the most superior performance, which might be ascribable to the satisfying dark adsorption capacity, efficient photocatalytic activity, ease of magnetic separation, and economic efficiency. These results indicated that the deposition of Fe2O3 into TiO2 nanotubes significantly enhanced the activity of Fe2O3, which was mainly ascribed to the Fe2O3-induced formation of staggered iron oxides@TiO2 band alignment and thus efficient separation of h+ and e−. Furthermore, the PL intensity and lifetime of the decay curve were considered as key criterions for the activity’s evaluation. Finally, the leaching tests and regeneration experiments were also performed, which illustrated the inhibited photodissolution compared with TiO2/Fe3O4 and stable cycling ability, enabling 1FeTi to be a promising magnetic material for photocatalytic water remediation.