The development of high-efficiency and low-cost new catalysts is an extremely attractive topic. In this study, two different matrix bentonite-modified fly ash catalysts were successfully prepared, and the compressive strength of the catalyst was studied by using unsaturated dynamic and static triaxial technology. The axial compressive strength of FC (fly ash catalysts added with Ca-based bentonite) was greater than that of FN (fly ash catalysts added with Na-based bentonite). The catalyst reached 978 kPa. The prepared catalyst was characterized by X-ray diffraction analysis, Fourier transform infrared spectroscopy, scanning electron microscopy, and specific surface area analysis (BET) of the catalyst. In addition, denitration performance of different catalysts was explored, and the reaction conditions were optimized. The results demonstrate that when the mixing ratio of fly ash and calcium-based bentonite in the FC is 4:1, the compressive strength is relatively high, and the denitration rate reaches about 82%.