Abstract: PBTPELiquid crystalline ionomer blends were synthesized by nanometer CaSO4 whiskers and liquid crystalline ionomer (LCI) blended with PBT and PE through melt blending. Thermal behavior, morphological structure, and mechanical properties of the blends were investigated by differential scanning calorimetry (DSC), FTIR imaging analysis, and tensile measurement. Results show that the crystallization temperature and crystallinity of PE phase are increaseing with the adding of LCI in the blends. The LCI surrounds nanometer CaSO4 whiskers, and the reduced disperse phase size enables a finely dispersing phase at matrix. The mechanical properties of the blends are optimized when a proper amount of LCI and nanometer CaSO4 whiskers (m(PBTPE)∶m(CaSO4)=100∶3) are added.