The magnetoelectric composites of spinel ferrite Ni0.75Zn0.25Fe2O4 (NZF) and BiFeO3 (BFO) with general formula xNi(0.75)Zn(0.25)Fe(2)O(4) + (1 - x)BiFeO3 (x = 0, 0.10, 0.20, and 0.30) have been prepared via hybrid processing route. Subsequently, the effects of addition of NZF on structural, dielectric, magnetic, magnetoelectric, and optical properties of BFO have been investigated, and significant enhancements have been observed in physical observables such as grain size, dielectric constant, magnetization, and polarization in ferroelectric hysteresis loops. The variation of magnetization with temperature indicates the presence of spin glass behavior along with the ferromagnetic component. The magnetoelectric coupling is found with a value of magnetocapacitance to be 4.6 % for 30 mol% addition of NZF. The optical properties of the composites are also studied using UV-Vis diffuse reflectance spectroscopy, Photoluminescence spectroscopy, and FTIR spectroscopy.