A transparent SiO2–Al2O3–LiF–YF3 glass ceramic doped with Nd3+ was fabricated by melt quenching and subsequent heating. X-ray diffraction and transmission electron microscope results demonstrated that orthorhombic β-YF3 nanocrystals with a mean size of 23 nm were homogeneously precipitated among the glass matrix. Confirmed by the energy dispersive x-ray spectroscopy measurements, the crystal-like absorption and emission of Nd3+ indicated the partition of Nd3+ into YF3 nanocrystals in the glass ceramic. Detailed characterizations of the Stark components of the 4I9/2, 4I11/2, and 4I13/2 manifolds were performed using the low temperature fluorescence spectra for 4F3/2→4I9/2, 4F3/2→4I11/2, and 4F3/2→4I13/2 transitions of Nd3+ in the glass ceramic. The stimulated emission cross sections of the 4F3/2→4I11/2 intermanifold transition and the 4F3/2(R1)→4I11/2(Y1) inter-Stark transition were determined to be 7.24×10-20- sup> and 11.55×10-20 cm2, respectively, being preferable to those of Nd3+-doped laser glasses and glass ceramic embedding (Pb,Cd)F2 nanocrystals.