Despite the promising advances in photodynamic therapy (PDT), it remains challenging to target and treat deepseated solid tumors effectively. Herein, we developed an organoplatinum(II) complex (Pt-TPE) with self-assembly properties for sonodynamic therapy (SDT). Pt-TPE forms a nanofiber network structure through Pt−Pt and π−π stacking interactions. Notably, under ultrasound (US), Pt-TPE demonstrates unique selfassembly-induced singlet oxygen ( 1 O 2 ) generation due to a significantly enhanced singlet−triplet intersystem crossing (ISC). This generation of 1 O 2 occurs exclusively in the self-assembled state of Pt-TPE. Additionally, Pt-TPE exhibits sono-cytotoxicity against cancer cells by impairing mitochondrial membrane potential (MMP), inhibiting glucose uptake, and aerobic glycolysis. Furthermore, US-activated Pt-TPE significantly inhibits deep solid tumors in mice, achieving remarkable therapeutic efficacy even at penetration depths greater than 10 cm. This study highlights the potential of self-assembled metal complexes to enhance the efficacy of SDT for treating deep tumors.