We report an observation of anomalous anisotropic magnetoresistance (AMR) in bilayered La1.2Sr1.8Mn2O7 single crystals. A giant AMR is found to be 80% under a magnetic field of 1 T near the metal-insulator transition temperature, where AMR is defined as AMR=[ρ(H⊥c)−ρ(H∥c)]/ρ(H⊥c)×100%, and ρ(H⊥c) and ρ(H∥c) are the resistivity with the magnetic field perpendicular and parallel to c-axis, respectively. The AMR effect shows strong temperature and magnetic field dependences, and indicates a close interrelation with the anisotropic field-tuned metal-insulator transition.
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