Cement production is the third largest source of nitrogen oxides (NOx), an air pollutant that poses a serious threat to the natural environment and human health. Reducing NOx emissions from cement production has become an urgent issue. This paper aims to explore and investigate more efficient denitrification processes to be applied in NOx reduction from precalciner. In this study, firstly, the flow field, temperature field, and component fraction in the precalciner are studied and analyzed using numerical simulation methods. Based on this, the influence of the reductant injection height and amount on the SNCR was studied by simulating the selective non-catalytic reduction (SNCR) process in the precalciner. The effect of natural gas on the NOx emissions from the precalciner was also investigated. The simulation results showed that, with the increase in height, the NOx concentration in the precalciner decreased, then increased, then decreased, and then increased again. The final NOx concentration at the exit position was 531.33 ppm. In the SNCR denitrification process, the reductant should be injected in the area where the precalciner height is 26–30 m so that the reductant can fully react with NOx and avoid the increase of ammonia escape. The NSR represents the ratio of reductant to NOx, and the results show that the larger the NSR is, the higher the denitrification rate is. However, as the NSR approaches 2, the denitrification rate slows down and the ammonia escape starts to increase. Therefore, according to the simulation results, the NSR should be kept between 1 and 1.6. The denitrification rate reached the maximum value of 42.62% at the optimal condition of 26 m of reductant injection height and 1.6 of NSR. Co-firing of natural gas with pulverized coal can effectively reduce the NOx generation in the furnace. The denitrification rate reached the maximum value of 32.15% when the natural gas injection amount was 10%. The simulation results of natural gas co-combustion and SNCR combined denitrification showed that combined denitrification was better than natural gas co-combustion or SNCR denitrification. Under the condition of NSR of 1 and natural gas injection of 10%, the denitrification rate increased by 29.83% and 31.64% compared to SNCR-only or co-combustion-only denitrification, reaching 61.98%, respectively. Moreover, less reductant is used in co-denitrification, so the problem of excessive ammonia emissions can be avoided. The results of this study provide useful guidance for denitrification process development and NOx reduction in cement production.