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Highlights Three‐component piezoelectric composites, with castor‐oil‐derived polyurethane (COPU) as the matrix, reinforced with barium titanate (BTO) microparticles (as the primary piezo‐active inclusion) and with multiwalled carbon nanotubes (MWCNTs) were synthesized. BTO content is varied (3, 12, and 25 vol%), while the MWCNTs content is maintained constant at 0.65 wt% (0.37 vol%) w.r.t. the COPU matrix. The addition of MWCNTs significantly enhances the piezoelectric strain coefficient (d33$$ {d}_{33} $$), relative dielectric constant (k/k0), and piezoelectric response, that is, open circuit voltage (VOC) of the piezo‐composites. The (COPU/MWCNTs)/25 vol% BTO composite gives a d33$$ {d}_{33} $$ value of 1.8 ± 0.1 pC/N, an increase of ~1.38 times compared to COPU/25 vol% BTO composite (with a d33$$ {d}_{33} $$ value of 1.3 ± 0.1 pC/N). The relative dielectric constant (k/k0) value of two‐component COPU/BTO (25.0 vol%) increased from 10.34 ± 0.06 to 11.15 ± 0.05 by addition of 0.65 wt% MWCNTs. A maximum open circuit voltage of ~19.6 V for three‐component (COPU/MWCNTs)/ 25 vol% BTO composite was obtained at 45 N load and at 5 Hz frequency. This value (VOC) is ~1.29 times higher compared to COPU/25 vol% BTO composite (with VOC ~ 15.2 V). The k/k0 and d33$$ {d}_{33} $$ values and elastic moduli obtained via experiments were further compared with those obtained from finite element analyses based on kinematic uniform boundary conditions (KUBC) and from Eshelby–Mori–Tanaka micromechanics extended to the domain of linear piezoelectric composites. Castor‐oil‐derived (COPU/MWCNTs/BTO) three‐component composites were synthesized Integration of MWCNTs enhances d33$$ {d}_{33} $$ by ~1.38 times for COPU/25 vol% BTO Elastic modulus and electrical conductivity increased with the addition of MWCNTs Computational predicted k/k0 and d33$$ {d}_{33} $$ values closely match to experimental data [ABSTRACT FROM AUTHOR]