Large single crystals of Aluminum-zincohposphate (AlZnPO4-DFT) with different morphology have been hydrothermally synthesized by using ethylenediamine (EDA) as structure-directing agent. The effects of crystallization conditions and gel compositions on products were investigated in detail. The pure phase with DFT structure could be obtained at 170 degrees C, while the competitive phase would appear when the crystallization temperature rises to 190 degrees C. The quality of AlZnPO4-DFT crystals enhances firstly and then deteriorates with the extension of crystallization duration from 20 h to 50 h. Moreover, the gel composition not only affects the size of the product, but also affects the morphology and quality of the product.