As a room-temperature multiferroic, BiFeO 3 has been intensively investigated for both magnetoelectric devices and non-volatile ferroelectric memory applications. [1][2][3] BiFeO 3 , having a rhombohedral unit cell, has antiferromagnetic, ferroelectric and ferroelastic order parameters. Since BiFeO 3 exhibits coupling between spontaneous electric polarization in the [111] direction and the (111) antiferromagnetic planes, control of the magnetic order can be achieved by ferroelectric domain reorientation resulting from polarization switching by an external electric fi eld. [ 4 ] This possibility of controlling the magnetism by an electric fi eld has been demonstrated at room temperature in single crystals [ 5 , 6 ] and thin fi lms. [ 4 , 7 ] In addition, BiFeO 3 has the largest remanent polarization ( P r ∼ 100 μ C cm − 2 ) along the [111] polar direction among all known ferroelectrics, [1][2][3] which is a promising feature as a lead-free material for ferroelectric random access memory (FeRAM). Utilizing the large remanent polarization of BiFeO 3 would enable further reduction of the cell size limited by conventional ferroelectrics such as BaTiO 3 and Pb(Zr,Ti)O 3 .Both magnetoelectric and ferroelectric memory devices have the same control knob: polarization switching by an applied electric fi eld. [1][2][3][4][5][6][7] Due to the rhombohedral symmetry of BiFeO 3 , there are four ferroelastic variances and three different polarization switching events: (1) 71 ° switching from r1 − to r3 + , (2) 109 ° switching from r1 − to r2 + (or r4 + ), and (3) 180 o switching from r1 − to r1 + (the superscript + and -stand for up and down polarization, respectively). Each switching path is coupled to a different reorientation of the BiFeO 3 unit cell, and hence different coupling to the magnetic order [ 4 ] as well as different magnitudes of switchable polarization. [ 8 , 9 ] A degradation of the ferroelectric properties of BiFeO 3 will result in losing controllability of magnetic order switching in magnetoelectric devices and capacity for information storage in ferroelectric memory devices. Especially, polarization fatigue [ 10 , 11 ] will directly restrict the reliability of the actual devices. Hence it is important to understand the intrinsic fatigue behavior of each polarization switching path in BiFeO 3 thin fi lms. In this communication, we report polarization fatigue in BiFeO 3 that depends on switching path, and propose a fatigue model which will broaden our understanding of the fatigue phenomenon in low-symmetry materials.Previously, there were reports on fatigue characteristics of rhombohedral ferroelectrics: ferroelastic domain evolution with polarization fatigue in textured fi lms [ 12 , 13 ] and ceramics [ 14 , 15 ] of PZN-PT, and orientation dependence showing (111)-oriented samples are more easily fatigued than (001)-oriented ones in PZN-PT [16][17][18] and BiFeO 3 . [ 19 ] In order to study the intrinsic behavior of switching-path dependent fatigue, it is crucial (1) to control a single polarization sw...