An ultrasonic method was developed to fabricate novel mesoporous TiO2 nanocrystals doped with a high concentration of N (N/TiO2). The nanocrystals were characterized by physicochemical methods including N2 physical adsorption/desorption, X-ray diffraction, X-ray photoelectron spectroscopy, photoluminescence spectroscopy, transmission electron microscopy, and UV-Vis diffuse reflectance spectroscopy. The photocatalytic degradation of dimethyl phthalate, a hazardous chemical in water, by the prepared N/TiO2 nanocrystals under visible light irradiation (400–660 nm) was investigated. The results show that N-doping efficiency under ultrasonic irradiation is 3.2 times higher than under typical conditions, and the produced TiO2 nanocrystals have mesoporous structure. N/TiO2 fabricated under ultrasound exhibited much higher efficiency for the degradation of dimethyl phthalate than that prepared under typical conditions. The high photocatalytic degradation activity of N/TiO2 fabricated under ultrasound is mainly attributed to its high N content effectively increasing its ability to absorb visible light. 采用超声波辐射法制备了具有介孔结构的高浓度氮掺杂TiO2纳米晶(N/TiO2). 采用N2物理吸附/X射线粉末衍射/X射线光电子能谱/透射电镜/光致发光谱和紫外-可见漫反射光谱等手段对N/TiO2进行了表征. 以波长为400–660 nm的可见光为光源, 以水体污染物邻苯二甲酸二甲酯为降解对象, 考察了不同制备方法对N/TiO2光催化性能的影响. 结果表明, 超声波辐射使氮掺杂浓度提高了2.2倍, 该法制备的N/TiO2同时具有较好的介孔结构, 表现了更高的光催化降解邻苯二甲酸二甲酯的活性. 其活性提高的主要原因是N/TiO2含有更高浓度的氮和对可见光具有更强的吸收能力. An ultrasonic method was developed to fabricate mesoporous TiO2 nanocrystals doped with high concentration of N. N doping causes strong visible light absorption and high photocatalytic activity towards degradation of dimethyl phthalate under visible light irradiation.