To meet the requirements of the rapid development of large-scale energy storage systems, "Beyond Li-ion battery (LIB)" systems are attracting more and more attention. [1][2][3][4][5] Among various alkali metals ion batteries, potassium-ion batteries (KIBs) exhibit many advantages for large-scale energy storage system applications including: [6,7] 1) the low manufacturing costs because of the natural abundance of their raw materials; 2) much lower redox potential of K/K + (−2.93 V vs standard hydrogen electrode) leading to higher open-circuit voltage and higher energy density compared with sodiumion batteries (SIBs). [8][9][10] According to the advantages and properties of low production costs and high energy density, the KIB is considered as a promising energy storage system for large-scale energy storage application. However, KIBs suffer from inferior cyclic stability and insufficient power density resulting from the structure collapse of electrode materials due to the bigger K + Constructing 2D heterostructure materials by stacking different 2D materials can combine the merits of the individual building blocks while eliminating their shortcomings. Dichalcogenides are attractive anodes for potassium-ion batteries (KIBs) due to their high theoretical capacity. However, the practical application of dichalcogenide is greatly hampered by the poor electrochemical performance due to sluggish kinetics of K + insertion and the electrode structure collapse resulting from the large K + insertion. Herein, heterostructures of 2D molybdenum dichalcogenide on 2D nitrogen-doped carbon (MoS 2 , MoSe 2 -on-NC) are prepared to boost their potassium storage performance. The unique 2D heterostructures possess built-in heterointerfaces, facilitating K + diffusion. The robust chemical bonds (CS, CSe, CMo bonds) enhance the mechanical strength of electrodes, thus suppressing the volume expansion. The 2D N-doped carbon nanosheets interconnected as a 3D structure offer a fast diffusion path for electrons. Benefitting from these merits, both the MoS 2 -on-NC and the MoSe 2 -on-NC exhibit unprecedented cycle life. Moreover, the electrochemical reaction mechanism of MoSe 2 is revealed during the process of potassiation and depotassiation.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.