We report a large and nonvolatile bipolar-electric-field-controlled magnetization at room temperature in a Co40Fe40B20/Pb(Mg1/3Nb2/3)0.7Ti0.3O3 structure, which exhibits an electric-field-controlled looplike magnetization. Investigations on the ferroelectric domains and crystal structures with in situ electric fields reveal that the effect is related to the combined action of 109° ferroelastic domain switching and the absence of magnetocrystalline anisotropy in Co40Fe40B20. This work provides a route to realize large and nonvolatile magnetoelectric coupling at room temperature and is significant for applications.