Nd∶CaYAlO4 single crystal fibers with different atom number fraction (0.25%, 0.50%, 0.75%, 1.00%) were grown by the micro-pull-down method. The crystal structure of the single crystal fiber was tested by X-ray diffraction (XRD), and the results show that the crystal structure is tetragonal. The polarization absorption and fluorescence spectra of Nd∶CaYAlO4 single crystal fibers were tested at room temperature, and the samples have strong absorption near 807 nm. Among them, the absorption of 1.00%Nd∶CaYAlO4absorption is the strongest, and the absorption coefficients for σ and π polarization are 4.20 and 4.06 cm-1, respectively. The strongest emission peaks of 1.00%Nd∶CaYAlO4 single crystal fiber are at 1 080 nm in both σ and π polarization. The emission bandwidths are 17.7 and 17.8 nm for σ and π polarization, respectively. The fluorescence lifetime of 0.25%, 0.50%, 0.75% and 1.00%Nd∶CaYAlO4 single crystal fibers are 129, 133, 135 and 140 μs, respectively, and no concentration quenching is observed. The results show that Nd∶CaYAlO4 single crystal fiber is a potential gain medium for ultrafast lasers.