Reversible orbital reconstruction driven by ferroelectric polarization modulates the magnetic performance of model ferroelectric/ferromagnetic heterostructures without onerous limitations. Mn-d(x2-y2) orbital occupancy and related interfacial exotic magnetic states are enhanced and weakened by negative and positive electric fields, respectively, filling the missing member-orbital in the mechanism of magnetoelectric coupling and advancing the application of orbitals to microelectronics.