Substantial waste of wool textiles, along with a lack of effective treatment technology, has resulted in a significant resource and environmental constraints. Integrating wasted wool textiles with polymer is an effective way to prepare lightweight structural materials, but the resulting properties is closely linked to the interfacial interaction. Here, we proposed an interfacial manipulation strategy to direct interfacial diffusion and aggregation of amide-based nucleating agents (WBG) in polypropylene (PP)/wool fiber (WF) composites. Accordingly, the branched WBG fibers were anchored onto the WF surface to construct an interlocking interface between WF and PP so as to strengthen the interfacial interaction. The formation and regulation mechanism of the branched WBG fibers were demonstrated. Benefited from mechanical interlocking and β-nucleating function of the branched WBG fibers, the interfacial interaction between the WF and PP matrix was enhanced while the formation numerous β-PP was cultivated, endowing the composite with excellent strength and ductility. To demonstrate the application potential of this strategy, waste wool textiles were alternately embedded between WBG-containing PP sheets to create an interlocking interfacial laminate with an exceptional combination of strength and toughness, which is important to upcycle waste wool textiles.