Potassium-ion batteries have been regarded as the potential alternatives to lithium-ion batteries (LIBs) due to the low cost, earth abundance, and low potential of K (−2.936 vs standard hydrogen electrode (SHE)). However, the lack of low-cost cathodes with high energy density and long cycle life always limits its application. In this work, high-energy layered P2-type hierarchical K 0.65 Fe 0.5 Mn 0.5 O 2 (P2-KFMO) microspheres, assembled by the primary nanoparticles, are fabricated via a modified solvent-thermal method. Benefiting from the unique microspheres with primary nanoparticles, the K + intercalation/deintercalation kinetics of P2-KFMO is greatly enhanced with a stabilized cathodic electrolyte interphase on the cathode. The P2-KFMO microsphere presents a highly reversible potassium storage capacity of 151 mAh g −1 at 20 mA g −1 , fast rate capability of 103 mAh g −1 at 100 mA g −1 , and long cycling stability with 78% capacity retention after 350 cycles. A full cell with P2-KFMO microspheres as cathode and hard carbon as anode is constructed, which exhibits long-term cycling stability (>80% of retention after 100 cycles). The present high-performance P2-KFMO microsphere cathode synthesized using earth-abundant elements provides a new cost-effective alternative to LIBs for large-scale energy storage.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10. 1002/adfm.201800219. in vain due to the limited and unevenly distributed Li sources. [2] In addition, the rapid expansion of renewable energy market from wind, solar, hydropower, and other intermittent energy sources has also triggered growing demand for high-energy density and low-cost energy storage systems, which further stimulated broad investigation beyond the Li-ion battery technologies. [3][4][5] Among these technologies, sodium-ion batteries (SIBs) and potassium-ion batteries (PIBs) are the two most promising alternatives to LIBs due to the earth-abundance and accessibility of Na and K compared with Li. [3][4][5][6][7][8] Statistically, K and Na elements remarkably occupy 2.09 and 2.3 wt% of the earth's crust (vs 0.0017% of Li) respectively. [3,9] However, since K has lower standard redox potential (−2.936 V vs standard hydrogen electrode (SHE)) than Na (−2.714 V), and is close to Li's potential (−3.040 V), a higher operating voltage, thus a high energy density could be delivered for PIBs, which seems to be a more attractive choice as affordable replacement of LIBs as large-scale energy storage system. [4,6,7] Extensive efforts have been devoted to explore high capacity PIB anode and significant advances have been achieved in high performance anode materials. [10][11][12][13][14][15][16][17][18][19] Among them, the carbonaceous materials (graphite, [10,13,14] hard/soft carbon, [12,13] and graphene [18] ) and metal (antimony, [19] tin [15] ) and metal oxides (K 2 Ti 4 O 9 ) [17] show very promising performance. Different from the wide range of options on anode materials, only a limited number...