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An ultrabroadband near-infrared (NIR) emission of Ni 2+ is demonstrated in a highly transparent nano-glass ceramic (nano-GC) containing Ga 2 O 3 nanocrystals with 808 nm excitation of Nd 3+. It is also shown that by adding Yb 3+ as an energy transfer (ET) bridge, the Ni 2+ emission could be substantially enhanced. The dopant distribution was studied using advanced analytical transmission electron microscopy. This, together with optical transmission measurements, steady-state and time-resolved emission spectra, is utilized to understand the underlying ET mechanisms between Nd 3+ , Yb 3+ , and Ni 2+. The feasibility of this device as a viable source is demonstrated using dual-laser pumping at 808 and 980 nm for the greatest Ni 2+ emission enhancement reported to date. The Nd 3+ /Yb 3+ /Ni 2+ triply doped nano-GC offers a promising gain medium for broadband and tunable NIR fiber amplifiers.