As a promising electrochemical energy device, a rechargeable zinc-air battery (RZAB) requires cost-effective cathode catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Some earth-abundant transition metal oxides have certain levels of bi-functional ORR/OER catalytic activities yet low electronic conductivities. The addition of high-electronic-conductivity material such as carbon black could result in another problem because there is low compatibility between metal oxide and carbon. In this work, polymer chains are ultrasonically prepared to act as binders to anchor metal-oxide active sites to porous domains of carbon black. The monomer N-isopropyl acrylamide is polymerized under ultrasonication instead of using conventional radical initiators which are dangerous and harmful. Reactive free radicals produced by ultrasonic irradiation can also help to form the Mn-Ni-Fe tri-metallic oxide. Thus, aided by the amide-type polymer as an adhesive, the tri-metallic oxide anchored on polymer-grafted carbon black prepared by ultrasonication possess a large number of metal-oxide active sites and hierarchical pores, contributing substantially to the enhanced ORR/OER electrocatalytic performance in the RZABs. Accordingly, this work provides interesting insight into the effective combination of inherently incompatible components for the fabrication of composite materials from an ultrasonic standpoint.