Ni‐rich cathode materials provide high energy density, but their structural and surface instability limits their cyclability and thermal stability. As one of the approaches to mitigate this problem, cathode materials comprising Ni‐rich high‐capacity core wrapped in Mn‐rich multiple shells are produced successfully. In contrast to the conventional batch‐type process for concentration‐gradient materials, a digital‐gradient cascade coprecipitation process described here achieves the improvements in productivity and quality consistency needed to move toward large‐scale manufacturing. The core–multishell cathode materials produced in this manner not only have longer cycle life and improved rate performance compared to homogeneous Ni‐rich cathode materials having the same overall composition, but also show remarkably enhanced thermal stability and low impedance growth characteristics. In a novel attempt to determine the correlation between the mechanical properties of the core–multishell cathode particles and their electrochemical cyclabilities, their breaking force and elasticity were successfully measured using a statistical approach, which indicates that a cathode particle with stable surface composition as well as high breaking force has improved capacity retention and durability. These results guide the realization of long life and high thermal stability in Ni‐rich cathode materials through heterogeneous particle engineering.