Cluster complexes with steady, effective, and broadband emission hold great promise for applications in bioimaging, sensing, optoelectronics, and lighting. The synthesis of such cluster complexes usually depends on solution processing and wet-chemical deposition approaches, which face considerable difficulties. To synthesize all-inorganic tellurium cluster in supercooled melts (e.g., Tellurium cluster-doped borate glass), the tellurium's morphology is fine-tuned by modifying the glass network topology and melting conditions in this paper. The experimental findings reveal that under a reducing atmosphere, integrating glass with a high degree of network polymerization and alumina dispersion effect regulates the size and shape of clusters to stably form near-infrared active D_2h-Te₄ clusters and achieve high-efficiency ultra-broadband near-infrared luminescence pumped by 808 nm laser in all-inorganic tellurium cluster D_2h-Te₄ doped borate glass.