Calix[4]arene-based chiral organocatalyst derived from L-proline supported onto well-defined (15 ± 3 nm) magnetic Fe<inf>3</inf>O<inf>4</inf> nanoparticles was used as a highly active, recoverable, and reusable catalyst for the asymmetric aldol reaction in water without need for organic solvents. The chiral organocatalyst showed high catalytic activity (up to 94%), enantioselectivity (up to 93%) and diastereoselectivity (up to 97:3) for the reaction between cyclohexanone and aromatic aldehydes. The catalyst could easily separated using an external magnetic field and reused for several times without any significant loss of activity.