A novel and general method is proposed to construct three-dimensional graphene/metal oxide nanoparticle hybrids. For the first time, it is demonstrated that this graphene-based composite with open pore structures can be used as the high-performance capacitive deionization (CDI) electrode materials, which outperform currently reported materials. This work will offer a promising way to develop highly effective CDI electrode materials. 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.

Three‐Dimensional Graphene/Metal Oxide Nanoparticle Hybrids for High‐Performance Capacitive Deionization of Saline Water