The present study focuses on improving the entanglement reconstruction of low-entanglement ultrahigh-molecularweight polyethylene (UHMWPE) through the incorporation of small particles into large particles in different sintering temperature environments. 10 wt % of small particles was added to the large particles, and the resulting entanglement degree of sintered products was examined through isothermal annealing experiments, high-temperature tensile tests, and rheological measurements. To gain insights into the entanglement formation process, the McLeish theory was employed to analyze the rheological results, and the chain dynamics of the bulk and interface domains in the particles were calculated. The analysis revealed that the addition of small particles significantly enhanced entanglement formation in both the interface and bulk domains of the particles. Regarding the characterization of the crystalline structures, it is found that the establishment of interphase has a positive correlation with entanglement construction, especially at a high sintering temperature. The tailored dimension of particle sizes and sintering temperatures result in optimized entanglement density and interphase content, leading to a substantial improvement in the tensile strength and breaking elongation of the material.