In this paper, we report a strategy for hybrid multiferroicity at nanoscale. Multiferroic NiFe2O4–Pb(Zr0.52Ti0.48)O3 composite nanofibers are synthesized by a sol-gel process and electrospinning, with fiber diameters ranging from 100 to 400 nm. Energy dispersive spectroscopy and transmission electron microscopy indicate that nanocrystalline Pb(Zr0.52Ti0.48)O3 and NiFe2O4 grains are randomly distributed in the composite nanofibers, with grain size around 30 nm. The spinel structure of NiFe2O4 and the perovskite structure of Pb(Zr0.52Ti0.48O3) are verified by x-ray diffraction, and multiferroicity of the nanofibers is confirmed by piezoresponse force microscopy and magnetic hysteresis. The structures and properties of the composite nanofibers are also compared with single-phase Pb(Zr0.52Ti0.48)O3 and NiFe2O4 nanofibers. These composite nanofibers could lead to unconventional multiferroic structures and devices.