By introducing high density polyethylene (HDPE) into the dispersed phase of impact polypropylene copolymers (IPCs), the morphologies of IPC/HDPE blends were regularly tailored and consequently the tensile and impact properties were simultaneously improved. Morphological observations showed a series of multilayered core-shell dispersed particles when the content of HDPE was less than 40%, while the continuous network structure was observed beyond 40%. With an increase in the content of HDPE, the size of the core increased and the number of dispersed particles with incomplete encapsulated polyethylene (PE) cores rose. More valid 'bridges' made up of segmented ethylene-propylene copolymer (sEbP) appeared and connected the PE core and polypropylene (PP) matrix. Meanwhile, co-crystallization occurred in the core phase, between long ethylene chain segments of the joined HDPE and sEbP in multi-component IPCs. The increased HDPE in blends reduced defective co-crystals, and in turn led to a thicker average lamellar thickness and thinner amorphous thickness of PE. Partial inserted ethylenepropylene random sequences are constrained by narrowed PE amorphous layers. Hence, the connection between the PP matrix and the dispersed phase was strengthened by co-crystals, 'bridges' and restriction effects. The tensile strength of the blends was slightly enhanced with an increase in HDPE, while the greatly improved toughness was achieved at a HDPE content of 30 wt% and kept constant with more HDPE. Thus, the interactions rather than core-shell phase morphology are regarded as the predominate factor for the excellent properties.