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Bicontinuous hierarchically porous Mn2O3 single crystals (BHP-Mn2O3-SCs) with uniform parallelepiped geometry and tunable sizes have been synthesized and used as anode materials for lithium-ion batteries (LIBs). The monodispersed BHP-Mn2O3-SCs exhibit high specific surface area and three dimensional interconnected bimodal mesoporosity throughout the entire crystal. Such hierarchical interpenetrating porous framework can not only provide a large number of active sites for Li ion insertion, but also good conductivity and short diffusion length for Li ions, leading to a high lithium storage capacity and enhanced rate capability. Furthermore, owing to their specific porosity, these BHP-Mn2O3-SCs as anode materials can accommodate the volume expansion/contraction that occurs with lithium insertion/extraction during discharge/charge processes, resulting in their good cycling performance. Our synthesized BHP-Mn2O3-SCs with a size of ~700 nm display the best electrochemical performance, with a large reversible capacity (845 mA h g(-1) at 100 mA g(-1) after 50 cycles), high coulombic efficiency (>95%), excellent cycling stability and superior rate capability (410 mA h g(-1) at 1 Ag(-1)). These values are among the highest reported for Mn2O3-based bulk solids and nanostructures. Also, electrochemical impedance spectroscopy study demonstrates that the BHP-Mn2O3-SCs are suitable for charge transfer at the electrode/electrolyte interface. ; This work was realized in the frame of a program for Changjiang Scholars and Innovative Research Team (IRT1169) of the Chinese Ministry of Education. B. L. Su acknowledges the Chinese Central Government for an "Expert of the State" position in the Program of the "Thousand Talents". Y. Li acknowledges Hubei Provincial Department of Education for the "Chutian Scholar" program. T. Hasan acknowledges funding from a Royal Academy of Engineering Research Fellowship and EPSRC IAA Grant (GRASS). This work is also financially supported by the Ph.D. Programs Foundation of Ministry of Education of China (20120143120019), This work is also financially supported by Hubei Provincial Natural Science Foundation (2014CFB160) and Self-determined and Innovative Research Funds of the SKLWUT (2015-ZD-7). We thank J.L. Xie, X.Q. Liu and T.T. Luo for TEM analysis from the Research and Test Center of Materials, Prof. L.Q. Mai for EIS analysis from WUT-Harvard Joint Nano Key Laboratory at Wuhan University of Technology. ; This is the final version of the article. It first appeared from NPG via http://dx.doi.org/10.1038/srep14686