Multiferroic nanostructures of Ni0.6Zn0.4Fe2O4-BaTiO3 (NZF/BT) have been prepared by two synthesis routes, i.e., chemical combustion (CNZF/BT) and hydrothermal (HNZF/BT). The synthesis of CNZF/BT results in nanoparticles of average size 4 nm at 500 °C annealing. However, the synthesis of HNZF/BT with hydrolysis temperature 180 °C/48 h shows nanowires of diameter 3 nm and length >150 nm. A growth mechanism in the fabrication of nanoparticles and wires is given. X-ray diffraction is used to identify the crystalline phase. The transmission electron microscopy shows the dimensions of NZF/BT nanostructures. The ferromagnetism, ferroelectricity, and magnetoelectric coupling show more enhancements in HNZF/BT nanowires than CNZF/BT nanoparticles. The observed polarization depends upon shape of nanostructures, tetragonal phase, and epitaxial strain. The tension induced by the surface curvature of nanowire counteracts the near-surface depolarizing effect and meanwhile leads to unusual enhancement of polarization. The ferromagnetism depends upon superficial spin canting, spin pinning of nanocomposite, and oxygen vacancy clusters. The magnetoelectric coefficient as the function of applied dc magnetizing field under ac magnetic field 5 Oe and frequency 1093 Hz is measured. The nanodimensions of NZF/BT are observed dielectric constant up to 120 MHz. The optical activity of NZF/BT nanostructures is shown by Fluorescence spectra.