Zeolitic imidazolate frameworks (ZIFs) were successfully prepared and applied in the environmentally friendly transfer hydrogenation of cinnamaldehyde to cinnamyl alcohol. This was proved to be a homogeneous reaction in heterogeneous system. The experimental results show that ZIFs have better catalytic performance than nitrate. To overcome the recycling of the catalysts, the hydrophobically modified core-shell structure ZIF-67@SiO2-CPTEOS was successfully prepared and hydrogenation took place in this core-shell structure as in a nanoreactor. The reaction rate was enhanced and the active site of the formed metal-N was confined in the core-shell structure nanoreactor. ZIF-67@SiO2-CPTEOS presents better catalytic performance and stability. Furthermore, DFT calculation results show that the activation energy barrier of CoAN in ZIF-67 is lower than that of metallic Co dissociated from Co (NO3)(2)center dot 6H(2)O, which further confirms that introduction of N and thus the formed CoAN bond in ZIF-67 presents higher catalytic activity than that of metal Co. Finally, a possible reaction mechanism is proposed. (C) 2019 Elsevier Inc. All rights reserved.