considered ideal solutions for achieving energy conversion and storage in a sustainable way. [2] Nowadays, the key challenges of using these technologies and devices lie in the developments of more efficient and stable electrode materials. For the electrochemical water splitting, due to the high overpotential and intrinsically sluggish reaction kinetics of the oxygen evolution reaction (OER), low-cost, high efficiency and stable earth-abundant electrocatalysts are required to enhance the energy conversion efficiency. [3] Similarly, the commercial graphite anode materials for LIBs have limited inherent theoretical capacity (≈372 mAh g −1 ), which cannot meet the requirements of high energy density batteries for rapidly growing smartphone, electrical vehicles, and aerospace applications. How to further improve the energy density of LIBs faces great challenges. Therefore, it is urgent to invent competitive multifunctional electrode nanomaterials with suitable components and architectures for highly efficient OER electrocatalysts and highperformance LIBs.Recently, iron-based oxides have been widely studied in the fields of energy storage and conversions owing to their high electrochemical activity, rich redox properties, natural abundance, and simple preparation. [4] However, the electrocatalytic activity of Fe-based oxides is highly dependent on theirThe development of high-efficiency, robust, and available electrode materials for oxygen evolution reaction (OER) and lithium-ion batteries (LIBs) is critical for clean and sustainable energy system but remains challenging. Herein, a unique yolk-shell structure of Fe 2 O 3 nanotube@hollow Co 9 S 8 nanocage@C is rationally prepared. In a prearranged sequence, the fabrication of Fe 2 O 3 nanotubes is followed by coating of zeolitic imidazolate framework (ZIF-67) layer, chemical etching of ZIF-67 by thioacetamide, and eventual annealing treatment. Benefiting from the hollow structures of Fe 2 O 3 nanotubes and Co 9 S 8 nanocages, the conductivity of carbon coating and the synergy effects between different components, the titled sample possesses abundant accessible active sites, favorable electron transfer rate, and exceptional reaction kinetics in the electrocatalysis. As a result, excellent electrocatalytic activity for alkaline OER is achieved, which delivers a low overpotential of 205 mV at the current density of 10 mA cm −2 along with the Tafel slope of 55 mV dec −1 . Moreover, this material exhibits excellent high-rate capability and excellent cycle life when employed as anode material of LIBs. This work provides a novel approach for the design and the construction of multifunctional electrode materials for energy conversion and storage.