To exploit the T2 weighted MRI performance of Fe3O4, and T1‐weighted MRI performance of Mn2+, Zhao and co‐workers constructed yolk–shell nanohybrids (Fe3O4@C/MnO2‐PGEA, PCMP) that were composed of Fe3O4 core, carbon interlayer, MnO2 shell, and a polycationic cloak.[24d] To induce effective tumor inhibition, the FCMP NPs catalyzed Fenton and Fenton‐like reactions to initiate multi‐augmented CDT, and reversed the highly immunosuppressive TME by Fe‐induced TAM polarization and Mn‐induced cGAS‐STING activation. This evidence concerns the gene CGAS and neoplasm.