Nanocrystalline glass ceramics with different concentrations of Nd3+-doped NaYF4 are prepared by melt quenching. Different characterization methods show that the cubic NaYF4 crystalline phase has been formed. Based on the absorption and emission spectra of samples, the absorption (σabs) and emission (σsem) cross sections of Nd3+ (4I9/2 ↔ 4F3/2) in the NaYF4 nanocrystalline glass ceramics are analyzed. The absorption and emission spectra show typical absorption and emission peaks, suggesting the possibility of concentration quenching. The values of σabs and σsem reach 2.04 × 10−21 cm2 and 1.93 × 10−21 cm2, respectively, which are comparable to those of other glasses, and a positive value of the gain cross section (σg) for 0.89 µm is obtained when the population inversion is chosen as 0.2. The results show that the studied material has promising applications in waveguide lasers and optical amplifiers.