Enriching the application of multifunctional dendritic mesoporous organosilica (DMOS) is still challenging in anti-cancer research. Herein, manganese ions, iron ions, or cobalt ions and tetrasulfide bonds are co-incorporated into the framework of DMOS to yield multifunctional nanoparticles denoted as Mn-DMOS, Fe-DMOS, or Co-DMOS by directly doping metal ions during the synthetic process. Due to co-incorporation of metal ions and tetrasulfide bonds, these designed nanocarriers have more functions rather than only for cargo delivery. As proof of concept, the nanocomposite is established based on Mn-DMOS as an efficient nanocarrier for indocyanine green (ICG) delivery and modification with polyethylene glycol. In the tumor microenvironment, the generated hydrogen sulfide (H