Silane pre-functionalized carbon dots, arbitrarily doped (0–100% scale) carbon dot nanohybrid gel glasses and macrostructures with high luminescence (quantum yields = 47% and 88%, respectively) and broadband optical limiting properties (532 and 1064 nm) are reported. These glasses are optically, thermally, and mechanically stable, as well as highly transmissive (ca. 90%) in the 400–1350 nm region.