Based on a specially designed optical structure, an efficient cascaded third-harmonic-generation (THG) output of a 1064-nm, pico-seconds pulse laser is successively realized by using an NH 4 H 2 PO 4 (ADP) crystal that acts as the secondharmonic-generation component and sum-frequency-generation component. The maximum THG output is 1.61 mJ, and the highest conversion efficiency from 1064 nm to 355 nm reaches 35%, which are obviously superior to the results obtained using a KDP crystal under the same circumstance. The further phase-matching analysis indicates that this THG configuration of ADP crystal can be applied to various fundamental wavelengths in a range of 1 Β΅m-1.1 Β΅m. Compared with the previously reported KDP THG converter, which is based on a similar principle, the present ADP THG converter is favorable for large-energy, high-efficiency operation because of the larger effective nonlinear optical coefficient d eff and higher laser damage threshold.