In this work, polyolefin-blend/clay nanocomposites based on low-density polyethylene (LDPE), linear low-density polyethylene (LLDPE), and organically modified clay (OC) were prepared by melt extrusion. Various grades of maleic anhydride (MA) grafted polyethylene (PE-g-MA) were used and examined as compatibilizers in these nanocomposites. Differential scanning calorimetry analysis showed that OC and compatibilizer affect the crystallization behavior of LDPE/LLDPE with different mechanisms. Thermodynamic calculations of wetting coefficient based on interfacial energy between OC, LD, and LL, Morphological characterization based on field emission scanning electron microscopy, X-ray diffraction, small angles X-ray scattering, and dynamic rheology measurements revealed that the compatibilizer and OC were localized at the interface of LDPE and LLDPE phases with a preferred tendency toward one phase. Results demonstrated that at a specific amount of OC, there is an optimum compatibilizer concentration to achieve nanodispersed OC and beyond that the compatibilizer causes a structural change in the polymer crystalline morphology. It was also found that the tensile property enhancement of LDPE/LLDPE/OC nanocomposites is closely related to the crystalline structure development made by incorporation of both OC and compatibilizer.