We present a resonant x-ray diffraction study of the magnetic order in NdFe 3 (BO 3 ) 4 and its coupling to applied electric fields. Our high-resolution measurements reveal a coexistence of two different magnetic phases, which can be triggered effectively by external electric fields. More in detail, the volume fraction of the collinear magnetic phase is found to strongly increase at the expense of helically ordered regions when an electric field is applied. These results confirm that the collinear magnetic phase is responsible for the ferroelectric polarization of NdFe 3 (BO 3 ) 4 and, more importantly, demonstrate that magnetic phase coexistence provides an alternative route towards materials with a strong magnetoelectric response. Frustrated magnetic materials exhibit a large variety of intriguing physical phenomena, including the concomitant appearance of coupled ferroelectric and magnetic orders [1,2]. In fact, interlinked magnetic and ferroelectric orders are very rare in nature. Their discovery in variety of frustrated magnets was therefore a surprise and generated a lot of excitement [3,4], not only because these phenomena are very interesting from the viewpoint of basic research. There is also a significant technological potential [5,6]. Especially since a strong magnetoelectric coupling enables to store information in an extremely energy efficient way [7,8]. Indeed, earlier experiments could demonstrate modifications of a magnetic order related to the reversal of the electric polarization [9][10][11]. These studies, however, were concerned with electric field induced changes within a single magnetic phase or the manipulation of phase stability close to a magnetic transition [12].In the present study we consider a different situation, where frustrated magnetic interactions cause two distinct ordered states to be metastable well below the observed critical temperatures, even in the absence of any first order transition. As a specific example, we investigated the electric field dependence of the magnetic order in NdFe 3 (BO 3 ) 4 , which is a frustrated magnetic material with a large magnetoelectric response [13]. We show that a small perturbation created by an applied electric field allows controlling the stability of the coexisting collinear and helical magnetic orders. This implies that phase coexistence driven by magnetic frustration underlies the magnetoelectric response of NdFe 3 (BO 3 ) 4 , providing an alternative route towards large magnetoelectric effects.The rhombohedral lattice structure of this material is illustrated in Fig. 1, where, for the sake of simplicity, only the two magnetic sublattices of Fe and Nd are shown. These two sublattices are magnetically coupled and undergo two magnetic phase transitions as a function of temperature [15][16][17]: upon cooling, commensurate magnetic (CM) order sets in first at T N ≈ 30 K. In this phase the spins are ordered in a collinear fashion, forming ferromagnetic (FM) ab-planes, which are coupled antiferromagnetically (AFM) along the c-direction. The ...