Abstract.A new synthetic approach has been developed to prepare α-Fe2O3@TiO2 core-shell nanostructures at ambient conditions (e.g., in water, ≤100 °C). This approach shows a few unique features, including: short reaction time (a few minutes) for forming core-shell nanostructures, no requirement of high temperature calcinations for generating TiO2 (e.g., at 80-100 °C), tunable TiO2 shell thickness, high yield and good reproducibility. The experimental results show that the α-Fe2O3@TiO2 core-shell nanostructures exhibit enhanced photocatalytic activity compared to the pure TiO2 (P25) and pure Fe2O3 in degradation of organic dye molecules with visible light irradiation. This could be attributed to the large surface area of TiO2 nanoparticles for maximum adsorption of dye molecules, and the effective charge separation at the heterojunction of α-Fe2O3 and TiO2. The findings may open a new strategy to synthesize TiO2-based photocatalysts with enhanced efficiency for environmental remediation applications.