A high-energy nickel-rich cathode with primary particle concentration gradient is developed via a simple, one-step process involving a sacrificial polymeric-bead cluster. The primary particles' gradients and internal buffer space in the secondary particles are successfully formed without any surface coating reagents. It is demonstrated that the cathode material has a high specific capacity and thermal stability. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.