Rod-shaped manganese dioxide (MnO
2) nanoparticles with three different crystallographic phases, namely α-, β-, and γ-MnO
2, were hydrothermally prepared. The products were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), Brunaure-Emmett-Teller (BET) method, and electrochemical measurements as cathode materials for secondary lithium-ion batteries. The crystalline phase of MnO
2 depended mainly on the Mn concentration of precursor solution and reaction temperature whereas it was not influenced by the pH value of precursor solution. All the samples were obtained as secondary particles composed of rod-shaped nanoparticles and the sizes of α- and γ-MnO
2 were smaller than that of β-MnO
2. In electrochemical tests, the γ-MnO
2 had the highest initial capacity of 190 mA h g
−1 among three different crystal phases and maintained better performance than the other crystallographic samples in the subsequent discharge/charge cycles. As a result, the electrochemical performance of MnO
2 depends on the crystal structure rather than the particle size.
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