Magnetoelectric (ME) multiferroic composites are more promising candidates for low-power consumption devices, next-generation spintronic devices, and multistate memory devices since they exhibit significantly higher Magnetoelectric interaction over single-phase multiferroics. In this regard magnetic behaviour, dielectric, and magnetoelectric characteristics of a novel Pb-free (1-x) Na0.5Bi0.5TiO3-(x) Ni0.5Co0.5Fe2O4, (x = 0, 0.2, 0.4, 0.6, 0.8 & 1) particulate composites were explored. Solid-state synthesis was adopted to prepare the single-phase Na0.5Bi0.5TiO3 (NBT), Ni0.5Co0.5Fe2O4 (NCFO), and their composites. The presence of rhombohedral NBT and cubic inverse spinel NCFO in the composites were confirmed with X-ray diffraction (XRD) patterns. Microstrain (ε) induced in the prepared samples was estimated by using the Williamson-Hall (W-H) method. The piezoelectric NBT phase shows the tensile strain and the ferromagnetic NCFO shows the comprehensive strain. Among all the composites 0.8NBT-0.2NCFO shows a higher strain value of 0.012%, and the decrement in the strain values was observed upon increases in ferrite concentration. Backscattered scanning electron microscope (BS-SEM) images revealed the existence of highly dense uniformly distributed elements and Energy dispersive spectroscopy (EDS) confirmed the existing elements in the composites. UV–vis absorbance spectra disclosed a rise in energy gap values from 1.14 eV to 3.0 eV with increasing NBT percentage. Variations of dielectric permittivity and dielectric loss with respect to AC frequency were studied at room temperature (RT), and the 0.2NBT-0.8NCFO sample shows a high dielectric permittivity of 8500 at ∼100Hz. M − H (Magnetization-Magnetic field) hysteresis loops demonstrate the pure ferrite phase has a coercive field (Hc) = 578 Oe, remnant magnetization (Mr) = 21.43 emu/g and saturation magnetization (Ms) = 71.29 emu/g. The Ms and Mr values in the composites are enhanced with increasing ferrite percentage. Studies on ME behaviour of (1-x) NBT-(x) NCFO, (x = 0.2,0.4,0.6 & 0.8) show the coupling effect between both the phases at room temperature and the highest coupling coefficient value 3.16mV/Cm. Oe was observed for the 0.8NBT-0.2NCFO further the reasons and mechanisms are discussed.