In article number 2000717, Qiaobao Zhang, Chenghao Yang, Jun Lu and co-workers demonstrate that the strategy of interfacial engineering via surface-amorphization of VO2 (B) nanorods results in the formation of a crystalline core/amorphous shell heterostructure. This design enables superior potassium-ion storage performance in terms of large capacity, outstanding rate capability and long cycle stability when employed as an anode for potassium-ion batteries.