Transition metal dissolution in layered cathodes is one of the most intractable issues that deteriorate the battery performance and lifetime. It not only aggravates the structure degradation in cathode but also damages the solid electrolyte interphase in anode and even induces the formation of lithium dendrites. In this work, we investigate the dissolution behaviors of polycrystalline and single-crystalline layered cathode via operando X-ray imaging techniques. The cathode particle morphology appears to have a significant impact on the evolution of the dissolution dynamics. As a mitigation strategy, we reveal that doping with a trace amount of Zr in the layered cathode could improve its robustness against the transition metal dissolution. Our finding provides valuable insights for designing the next-generation highly stable layered battery cathodes.