Nitrogen oxide (NOx) is one of the world's major air pollutants. Thus, utilizing inexpensive mineral materials to develop an efficient and low-temperature denitrification catalyst is of great significance. In the present work, palygorskite (Pal)-supported perovskite-type LaFe1-xNixO3 (x = 0.1-0.9) nanocomposites are prepared by a facile sol-gel method. Extensive tests are employed to characterize the textural and structural properties of samples. It is determined that perovskite particles are well dispersed on the surface of Pal with excellent NH3 adsorption. The impacts of various Ni doping on the NOx conversion under visible light irradiation are investigated. Results indicate that when x is less than 0.4, LaFe1-xNixO3 remains a perovskite solid solution supported uniformly on the Pal surface. When x is beyond 0.4, LaNiO3 phase co-precipitates and forms a coherent heterojunction of LaNiO3/LaFe0.6Ni0.4O3 on Pal. Photo-assisted selected catalytic reduction (Photo-SCR) of NO results show that the denitrification performance varies with the Ni content, and more than 90% of NO molecules can be reduced when x = 0.5 in low temperature range of 150-250 degrees C.