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The polyetherimide (PEI) that contained the well-dispersed fillers, multi-wall carbon nanotubes (MWNTs) and (Ba0.8Sr0.2) (Ti0.9Zr0.1)O3 ceramic powder (BSTZ), were prepared to investigate the composites with higher dielectric constants. Organic acids were covalently bonded onto the π-conjugated skeleton of the surface-modified MWCNTs by treating them with carboxylic acids. Analyses of Raman spectra of MWNTs demonstrated that the acid-treated process increased the number of defects in the graphitic layers. The dielectric properties of the MWNTs/PEI and MWNTs/BSTZ/ PEI composites with various MWNTs and BSTZ contents were developed under different frequencies. The Lichtenecker logarithmic mixing rule was used to find the effective dielectric constant of MWNTs and to predict the dielectric constants of the MWNTs/BSTZ/PEI composites.