Photonic media containing hybrid noble metal–dielectric nanocrystals (NCs) represent a wonderland of nanophotonics, with a myriad of uncharted optical functions yet to be explored. Capitalizing on the unique phase separation and spontaneous formation of Au-metal NCs in a gallosilicate glass, we fabricated
Ni
2
+
-doped transparent nanoglass composites (GCs) containing
Au
-
metal
/
γ
-
Ga
2
O
3
-dielectric NCs. Compared with GCs free of Au-metal NCs, the superbroadband near-infrared emission of
Ni
2
+
with a full width at half-maximum over 280 nm is enhanced twice in the
Au
-
metal
/
γ
-
Ga
2
O
3
dual-phase GCs. A comparison is given as to the spontaneous emission (SPE) properties of
Ni
2
+
in the dual-phase GCs when pumped resonantly and off-resonantly with the localized surface plasmon resonance band of the Au-metal NCs. The important role of the Au-metal NCs in the SPE enhancement is revealed by theoretical simulation based on the finite-element method. Combining the photonic engineering effect of hybrid
Au
-
metal
/
γ
-
Ga
2
O
3
NCs and the sensitization effect of
Yb
3
+
on
Ni
2
+
, a record-high enhancement factor of over 10 of the
Ni
2
+
NIR emission is achieved, and optical gain is demonstrated in the GCs at the fiber communication wavelength.
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