and the oxygen evolution reaction (OER) during the discharge/charge processes. [2] It is evident that an efficient catalyst can not only accelerate the lagging reaction kinetics, but also can avoid side reactions to deliver long-term stability. Therefore, exploring ideal catalysts plays a pivotal role in promoting the development of LOBs and is an urgent necessity. [3] Recently, noble metals and their alloys have exhibited excellent electrocatalytic activities toward the OER and ORR, but the high cost and scarcity of these electrocatalysts have seriously limited their commercial application. [4] Transition metal dichalcogenides (TMDs) have been attracting extensive attention worldwide on account of their low cost, excellent chemically active electrocatalytic property, and diversity of structure, so they have realized numerous applications in energy conversion and storage, including hydrogen evolution, batteries, and supercapacitors. [5] MoS 2 has become the most outstanding choice and has been widely applied in various fields due to its excellent catalytic activity. [6] Its application in the ORR/OER has been limited, however, by its low electrical conductivity and limited number of active sites. To this end, various feasible tactics have been employed to promote the electrochemical performance of MoS 2 in LOBs, such as combining with conductive Developing an excellent bifunctional catalyst is essential for the commercial application of Li-O 2 batteries. Heterostructures exhibit great application potential in the field of energy catalysis because of the accelerated charge transfer and increased active sites on their surfaces. In this work, CoS 2 nanoparticles decorated on MoS 2 nanorods are constructed and act as a superior cathode catalyst for Li-O 2 batteries. Coupling MoS 2 and CoS 2 can not only synergistically enhance their electrical conductivity and electrochemical activity, but also promote the heteroepitaxial growth of discharge products on the heterojunction interfaces, thus delivering high discharge capacity, stable cycle performance, and good rate capability.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202105752.