pulses as short as 10 ns, representing its great potential in high-speed nonvolatile memories. [14] For further improving the memory density, reducing the sample size has some limitations in precise processing and heat dissipation. To avoid these problems, multilevel storage that allows each unit to store multiple bits of information has been proposed. [15] Lately, multilevel polarization states have been discovered in various ferroelectric materials, such as Pb(Zr,Ti)O 3 (PZT) and BFO. [16,17] Based on the thickness-dependent ferroelectric domain size scaling behaviors, the formation of nanometer scale domains in very thin ferroelectric films can lead to the incomplete inversion of polarization. Various proportions of upward and downward polarization combined with the contribution from interfacial defect states can give rise to a continuous change of the interfacial barrier, which forms the basis of the multilevel storage.BFO is one of the most potential lead-free ferroelectric materials and the unique singular room-temperature multiferroic material. [18][19][20][21][22] Moreover, BFO is particular for its relatively narrow bandgap (<2.8 eV), which supports the PV effect in the visible range. [23,24] Recently, tetragonal-like BiFeO 3 (T-BFO) films, which has a giant axial ratio (c/a ≈1.24) has been demonstrated to be with a large polarization up to 150 µC cm −2 . [25,26] The discovery of such a large polarization in highly strained BFO thin films has attracted much attention for its great potential in nonvolatile information storages. Up to now, some methods such as nonidentical amplitude/width pulses or compliance current control have been employed to obtain the multilevel resistance. However, these solutions are not practical for high-frequency operation owing to extra programming time. [27] Since not only the electric field but also the PV effect can change the interfacial barrier of the heterostructure, it is possible to generate multiple resistance states (RS) with identical voltage and photopulses in a system where the PV and multilevel resistance effects coexist. Such photoassisted electric field modulation can be technically compatible with high-frequency manipulation. Wang et al. have reported the four resistance states in BFO-based heterostructures, which require two kind of reading procedures with laser illumination on and off. [10] However, the electrophoto double-modulated multiple nonvolatile resistance states that can be distinguishable by the same reading operation are still absent.For developing the high-density and high-speed nonvolatile memory storage, the photoassisted electric field modulation of resistive switching in ferroelectric heterostructures is studied. Highly strained epitaxial BiFeO 3 heterostructures are fabricated on LaAlO 3 substrates by magnetron sputtering. The electric field-modulated wide range multilevel resistance and switchable photovoltaic effects are observed in these heterostructures. It is found that the electric field-modulated interfacial barrier can be further affe...