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The importance of ZT in thermoelectric (TE) materials is critical for green power generation and cooling applications. Therefore, tremendous efforts were underway to improve ZT, in which we proposed a layer structured approach by successively arranging of coarse Bi 0.5 Sb 1.5 Te 3 (BST) and fine BST/0.07Cu microstructure materials and investigated their transportation mechanism. The dual bulk microstructure was well-bonded and confirmed by analyzing the microstructure through scanning electron microscope (SEM), electron backscatter diffraction analysis (EBSD) and simulated the electrical potential and temperature distribution during spark plasma sintering with COMSOL software. The results indicate that the highest power factor of 3.8 mW/m-K2 was attained in the layer structured sample, which is significantly higher than other samples due to its synergistically optimized electrical conductivity and Seebeck coefficient. Through the varied microstructure, the κ was decreased at 400 K and consequently the ZT was improved to 1.25 at 400 K for the layer structure samples. Therefore, it is suggested that layered arrangement of different microstructure material could improve the thermoelectric properties of materials. [Display omitted] • Novel fabrication of hierarchical structured material with successive arrangement of two different microstructures. • Successful consolidation of well-bonded hierarchical material and confirming by simulating results from COMSOL software. • Highest power factor of 3.8 * 10−3 W/m-K2 obtained by transportation of charge carriers through two different energy levels. • Hierarchical structured sample show highest figure of merit of 1.25 at 400 K which is highest among all reported samples. [ABSTRACT FROM AUTHOR]