A single crystal of 1% Er3+-doped CaYAlO4 has been grown by the traditional Czochralski method. The as-grown crystal showed optical transparency and developed two planes along the (001) direction. The absorption spectra showed a marked difference in the 4I15/2 → 4I13/2 and 4I15/2 → 4F9/2 transitions with different polarizing direction. Due to the disordered crystal structure, broad absorption, and emission spectra around 1550 nm were obtained. In our experiments, the lifetime of the 4I13/2 excited state of Er3+ was determined to be 3.46 ms by the powder method, while it was 4.95 ms in the bulk samples. In addition, the upconversion spectrum in the green and red regions was observed pumped by a laser diode (LD) at 970 nm.