Nanohybrid materials based on polyamino acids immobilized onto inorganic materials are of interest for their potential applications in protein engineering, biomedicine and catalysis. We developed an efficient and eco-friendly new protocol for the immobilization of synthesized poly-L-leucine (PLL) onto rehydrated hydrotalcite (HTr). To do this, we synthesized different PLLs containing both C-terminal and N-terminal groups and compared them with a commercial PLLc. These synthetic polypeptides were immobilized onto HTr in water as the liquid medium with less than 30 min of ultrasound treatment. The obtained PLLs/HTr synzyme showed excellent activity and enantioselectivity when used as a catalyst in the asymmetric Julia-Colonna epoxidation reaction of chalcone. Moreover, these nanohybrid materials based on PLLs did not require any pre-activation time, which were easily separated from the reaction media and, unlike the commercial PLLc-supported catalyst, were reusable, exhibiting high stability after five consecutive runs without any apparent deactivation. (C) 2011 Elsevier Inc. All rights reserved.