AbstractTuning the optical properties of active species embedded within a glass matrix by modifying the ligand environment is of interest for luminescence‐based technologies, for example, in optical sensing, data transmission, or spectral conversion. Here, we discuss a facile synthesis procedure for a glass‐crystal composite material comprising of bismuth (Bi)‐doped zirconia within an aluminoborate glass phase. The approach offers tunable and broad photoemission characteristics in the visible spectral region from 400 to 750 nm. Incorporation of Bi ions into the crystal phase enhances the photoemission intensity by two orders of magnitude, with an external quantum efficiency of about 29%. At higher ZrO₂ dopant concentration, we observe a red‐shift of both the excitation and the emission bands to match commodity ultra‐violet light emitting diodes as excitation sources. Encapsulation within the aluminoborate glass phase provides advantageous thermal behavior, with the emission intensity remaining at >80 % of its initial value up to a temperature of 400 K.