In this work, we reported the fabrication and magnetoelectric coupling properties of the multiferroic CoFe2O4-PbZr0.2Ti0.8O3(CFO-PZT) coaxial nanofibers synthesized by electrospinning technique. The coaxial structure of nanofibers was demonstrated by magnetic force microscope and transmission electron microscope. The multiferroic properties of coaxial nanofibers have been revealed by magnetic hysteresis loops and piezoresponse amplitude butterfly curves and phase hysteresis loops. The as-prepared coaxial nanofibers show an effective piezoelectric coefficientd(33)of 30 pm/V and a saturated magnetization of 12 emu/g. Their magnetoelectric response has been probed by means of the localized changes in magnetization after poling the domains of the composite system. A static, large converse magnetoelectric coupling coefficient of 1.2 x 10(-8) s/m was obtained in a single CFO-PZT nanofiber.