Atomic Ce‐Induced Adaptive Synergism for Self‐Optimized Multi‐Enzymatic Nanozyme Design for Soil Amendment

Abstract Single‐atom nanozymes (SAzymes) offer exceptional promise as next‐generation substitutes for natural enzymes due to its superior catalytic performance. However, single active sites of SAzymes have predominantly been limited to mimicking a monofunctional enzymatic activity, which hinders their adaptability in complex biological systems. Herein, an innovative Ce‐induced adaptive synergism is reported, which allows Ce single‐atom to activate Ni–Fe dual‐site adaptive synergy for boosting multi‐enzymatic activities of Ce‐modified nanozyme (Ce‐MOF), along with finely tuned reactive oxygen species (ROS) production. In‐situ spectroscopic studies and theoretical calculations reveal that Ce induces spin‐state polarization of Ni and Fe centers, promoting the generation of bound Ni/Fe = O intermediates that modulate ROS pathways depending on substrate and pH. This adaptive synergism enables continuous structural adaptation of the dual‐metal active sites, enhancing both catalytic efficiency and selectivity. Functionally, Ce‐MOF exhibits potent antifungal activity against Fusarium solani in vitro without the introduction of exogenous O2 or H2O2. Meanwhile, soil experiments demonstrate effective inhibition of phytopathogen colonization and a notable recovery of beneficial microbial communities via selective production of ROS. Furthermore, the amended soil treated with Ce‐MOF flourishes Panax ginseng growth and provides a promising solution for sustainable plant cultivation via rhizosphere microbiome regulation.