Core-shell nanofibers of nickel ferrite and lead zirconate titanate have been synthesized by electrospinning, assembled into superstructure in uniform or non-uniform magnetic fields, and have been characterized in terms of ferroic order parameters and strain mediated magneto-electric (ME) coupling. The core-shell structure was confirmed by electron microscopy and scanning probe microscopy. Studies on magnetic field induced polarization P in assembled samples showed a decrease or increase in P, depending on the nature of fibers and strengthening of ME coupling with change in remnant-P as high as 32%. Strong ME interactions were evident from H-induced variation in permittivity at 20-22GHz. (C) 2014 AIP Publishing LLC.