Ultrasonic technology has been intensively studied recently due to its special features. In this paper, an ultrasonic crystallization method was introduced for the preparation of ZnAl-Hydrotalcite-Like compounds (ZnAl-HTLcs). Samples with high crystallinity, small particle size and narrow particle size distribution were obtained and fully characterized using conventional techniques of XRD, FT-IR and TG-DTA. The results prove that both ultrasonic frequency and ultrasonic power have effects on the sizes of the product particles. By varying the ultrasonic power from 250 W to 88 W, with the ultrasonic frequency fixed at 59 kHz, the median particle size of the samples increased from 0.37μm to 0.82μm. By altering the hydrothermal treatment time from 1 h to 5 h at 110 ℃, the median particle size of ZnAl-HTLcs synthesized via ultrasonic crystallization increased from 0.88 μm to 1.11 μm.