The removal of Pb(II) from aqueous solutions was investigated using kaolin with two different particle sizes (2.3 and 45 μm) with and without nanoscale zero-valent iron (nZVI, at a Fe content close to 30%). The experimental results show that 2.3 μm kaolin loaded with nZVI (K-nZVI) had the best Pb(II) removal performance under various test conditions. After 24 h, it removed 99.5% of Pb(II) ions in the solution, followed by 45 μm K-nZVI, 2.3 μm kaolin, and 45 μm kaolin (89.01%, 68.8%, and 65.8%, respectively). The removal rates by all four kaolin samples increased with increasing pH in the range of 2-6, and with increasing temperature between 30°C-60°C. The results show that using finer carrier particles improves the performance of K-nZVI for removing Pb(II) in aqueous solutions.