The Neodymium (Nd) substituted Sr-based Z-Hexaferrites having composition Sr3-xNdxCo2Fe24O41 (x = 0, 0.15, 0.30 and 0.45) corresponding to pristine, 5, 10 and 15% substitution were prepared using solid-state reaction method in pre-optimized rare Earth metal solubility range (x ≤ 0.45) and labeled as SCFO, SNCFO5, SNCFO10 and SNCFO15, respectively. X-ray diffractometer and Scanning Electron Microscopy (SEM) were utilized to investigate the prepared samples’ structure and grain morphology. The X-ray diffraction (XRD) patterns confirmed Z-hexaferrite formation with adequate phase purity. Dielectric measurements exhibited a relaxation-type, frequency-dependent, and thermally activated dielectric response across all prepared samples. In Nd substituted SCFO, the obtained value of coercivity (Hc) ranges from 52.2–68.45 oersted, confirming a soft magnetic behavior. Magnetoelectric coupling coefficient(α) recorded at room temperature has a maximum value of 0.2133 mV cm−1Oe−1 for the pristine sample and this value of α varies with Nd substitution for all prepared samples.