[Introduction]The peeling layer is crucial for the successful fabrication and application of carrier-attached ultrathin copper foil.However,both single organic and inorganic peeling layers have their shortcomings.It is necessary to develop an inorganic-organic composite peeling layer to achieve the differential control of peel strength at multiple interfaces of carrier foil,peeling layer,and ultrathin copper foil.[Method]Firstly,a 35 μm-thick copper foil was prepared by electrodeposition as carrier.Secondly,an inorganic-organic composite peeling layer was fabricated by electrodeposition of Zn-Ni alloy layer and immersion in 2-mercaptobenzimidazole(2-MBI)successively.Finally,a carrier-attached ultrathin copper foil was obtained by electrodepositing an ultrathin copper foil onto the composite peeling layer.[Result]2-MBI molecules could be anchored onto the surface of Zn-Ni alloy layer through the bonding between N and S atoms with Zn and Ni,forming a Zn-Ni alloy/2-MBI composite peeling layer.The peel strength between the carrier foil and the ultrathin copper foil was moderate(about 0.083 N/mm)due to the presence of the composite peeling layer,and no Zn-Ni alloy layer would be left on the shiny side of the ultrathin copper foil after peeling.[Conclusion]The novel inorganic/organic composite peeling layer enables the differential control over the peel strengths of different interfaces in the carrier foil/peeling layer/ultrathin copper foil sandwich structure,laying the foundation for the successful fabrication of carrier-attached ultrathin copper foil.