COMMUNICATION 1800119 (1 of 8) © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.small-methods.com Rational Design of Hierarchical TiO 2 /Epitaxially Aligned MoS 2 –Carbon Coupled Interface Nanosheets Core/Shell Architecture for Ultrastable Sodium-Ion and Lithium–Sulfur Batteries Yong Yang, Shitong Wang, Sen Lin, Yutong Li, Weiyu Zhang, Yuguang Chao, Mingchuan Luo, Yi Xing, Kai Wang, Chao Yang, Peng Zhou, Yelong Zhang, Zilong Tang, and Shaojun Guo* DOI: 10.1002/smtd.201800119 With the coming of the “energy internet,” the pursuit of ultralong-life electrode mate- rials has triggered the unprecedented scien- tific research toward novel energy storage systems, instead of the conventional lithium-ion batteries (LIBs). Owing to the limited Li resources and unsatisfactory poor cycling performance, [1–4] the develop- ment of high-capacity electrode materials with ultrastable cycling performance is the key for the next generation of energy storage battery. To this end, sodium-ion batteries (SIBs) and lithium–sulfur (Li–S) batteries are emerging as competitive alternatives because of the abundant resources of Na and S. [5–8] Great effort have been devoted to exploring new electrode materials in SIBs. [9] Among them, titanium dioxide (TiO 2 ) has been intensively studied as anode material for SIBs, due to its relatively little volume expansion. [10–12] Never- theless, its slow sodium diffusion and relatively low intrinsic electronic conduc- tivity hinder its implementation in SIBs, The development of electrode materials with superior cycling stability is currently receiving intensive research for next-generation portable elec- tronic equipment. Herein, a novel 3D hierarchical architecture composed of TiO 2 /epitaxially aligned MoS 2 –carbon coupled interface nanosheets is reported for boosting sodium-ion storage and lithium–sulfur batteries, in which the MoS 2 nanosheets are epitaxially aligned grown on the surface of carbon nanosheets through a simple calculation conversion process. The resulting hybrid demonstrates ultralong-life performance for sodium-ion storage and lithium–sulfur batteries, owing to synergistic effects among the stable TiO 2 nanowires, the high-conductivity carbon nanosheets, and the vertical MoS 2 nanostructure. Even at a high current density of 8 A g -1 , the capacity can be maintained at 169 mA h g -1 after 15 000 cycles, one of the highest values for TiO 2 -based electrodes. Moreover, such peculiar sheet-on- sheet structure also brings benefits for lithium–sulfur batteries, providing an effective physical shield against polysulfide shuttling and chemical adsorption of polysulfides, with a low fading rate (0.039% per cycle over 1500 cycles). The present work highlights that this rationally designed hybrid nanoarchitecture is an effective strategy to boost the stability of electrochemical energy storage. Sodium-Ion Storage Dr. Y. Yang, Dr. W. Zhang, Dr. Y. Chao, Dr. M. Luo, Dr. Y. Xing, Dr. K. Wang, Dr. C. Yang, Dr. P. Zhou, Dr. Y. Zhang, Prof. S. Guo Department of Materials Science and Engineering College of Engineering Peking University Beijing 100871, China E-mail: guosj@pku.edu.cn Dr. S. Wang, Dr. Y. Li, Prof. Z. Tang State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084, China The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smtd.201800119. Dr. S. Lin State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and Technology Shanghai 200237, China Prof. S. Guo BIC-ESAT College of Engineering Peking University Beijing 100871, China Small Methods 2018, 1800119