The influences of roasting activation on the particle morphology, microscopic structure, and adsorption properties of natural clinoptilolites were investigated. The experimental results show that the optimal modified conditions include a calcination temperature at 400℃, a roasting time of 0.5 h, and furnace cooling. The ammonia nitrogen removal rate from analog renewable water of the modified clinoptilolites reached 72%in the optimized conditions, which is 12%higher than that of natural ones. Scanning electron microscopy analysis showed that the surface morphology changed, the micro-hole size increased, and the surface became smoother and more uniform after calcination. The single-point total adsorption average pore width increased from 7.74 nm to 10.64 nm.