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High dielectric constant BaTiO₃/ethyl cellulose (BT/EC) nanocomposites having BT loadings of up to 13 vol% were fabricated through a simple casting technique. The BT filler powder, synthesized through an ultrasonic‐assisted solid‐state route, was revealed by X‐ray powder diffractometry (XRD) and Raman spectroscopy to be dominantly tetragonal. Scanning electron microscopy (SEM) showed good dispersion of the BT nanoparticles in the EC polymer matrix at lower BT concentrations. However, at higher concentrations, the BT particles form a continuous phase or a “filler network” leading to weak BT/EC interactions. This finding is well supported by the results of the tensile strength and storage modulus. The dielectric properties of the BT/EC nanocomposites were investigated over wide ranges of frequency and temperature. The addition of BT significantly increased the permittivity (ε′) and dielectric loss (ε …