This is the first study to showcase the use of maleic anhydride‐grafted polyethylene (MAPE) to compatibilize polyethylene (PE)‐rich blends, where polypropylene (PP) represents the minor phase. By first mixing PP with MAPE, and then adding PE, MAPE was assumed to be localized at the PE/PP interface. Microscopy analysis confirmed that MAPE led to a remarkably fine PE/PP/MAPE morphology, with PP being uniformly dispersed into PE and having an average diameter 267% smaller than that in the PE/PP blend. According to mechanical and rheological tests, this translated into a 14%, 20%, and 14% enhancement of tensile strength, tensile modulus, and tensile toughness, respectively, as well as a 10% and 20% drop in PE/PP viscosity mismatch and interfacial tension, respectively. Finally, PE/PP/MAPE tensile toughness and elongation at break were greater than those of virgin PP, while PE/PP/MAPE strength and stiffness were similar to the ones of neat PP. Therefore, this study provides industries with the possibility to utilize products rich in PE instead of those made of more expensive PP, while still keeping the level of performance high; hence, creating a paradigm shift in the development of advanced lightweight polyolefin materials with tuned functionalities.