A comparative study of spectral-luminescent and Judd–Ofelt analysis of photo-thermo-refractive (PTR) glasses doped with a variable content of neodymium (0.5–2.11 mol%) has been carried out for the first time. The change of Judd-Ofelt parameters (Ω2, Ω4, Ω6), radiation lifetime, experimental lifetime, branching ratio and emission cross sections were demonstrated as a function of Nd2O3 concentration and compared to the equivalent parameters in other works. It was found that the 4F3/2 → 4I11/2 transition is enhanced in Nd-doped PTR glass. The quantum efficiency of 0.5 mol% Nd-PTR for the same transition is 90.3% and the induced emission cross section is 1.743 × 10−20 cm2. The saturation intensity for 4F3/2 → 4I11/2 laser transition in the same sample is 20.62 kW/cm2, it is lower than that in some commercially produced glasses of same Nd3+-concentration. Laser action of a 0.5 mol% Nd-PTR was demonstrated, it was found that the round-trip loss of this gain medium is 0.34%, this value is quite low, and it is comparable to that in some commercially fabricated Nd-YAG crystals.