The use of magnetic lanthanum-based materials for phosphate removal from river water has gained increasing attention. However, challenges to produce and use lanthanum-based materials in large-scale or pilot-scale studies remain. In this work, a kilogram-scale Fe3O4/La(OH)3 magnetically recyclable composite for removing phosphate from river water was developed through a low-temperature precipitation route. The composite was used to remove phosphate from river water at both bench- and pilot-scales. Based on the bench-scale tests, the developed Fe3O4/La(OH)3 composite was found to have excellent magnetic particle separation efficiency (>98%) and a sorption capacity of 11.77 mg/g for phosphate. A 1.0 g/L dosage of the composite in the river water sample was able to selectively reduce the phosphate level from 0.089 to 0.005 mg/L in 60 min over five consecutive adsorption cycles. At the pilot-scale, the Fe3O4/La(OH)3 composite only achieved 36.0% phosphate removal efficiency, which is considerably different from the bench-scale results over an operational time of five months and a total treatment volume of 300 m3. This significantly reduced removal efficiency is mainly attributable to turbidity, suspended solids, and organic matter in the river water and the deteriorated magnetic separation efficiency. This study revealed potential challenges and shed new insights on moving magnetic nanocomposite-based technology from the bench-scale to the pilot-scale, which can inspire new designs for the application of similar technology.