Taking high nitrogen aluminum dross as the research object, the effects of the additives sodium carbonate and cryolite and the roasting process on the denitrification effect of aluminum dross were studied. The principle of additive denitrification was studied by XRD, SEM and TG-DSC. The experimental results show that sodium carbonate and cryolite can quickly reduce the content of aluminum nitride in aluminum dross. The optimum denitrification process parameters were also obtained simultaneously. When the mass ratio of cryolite to aluminum dross was 0.4, the roasting temperature was 900 °C, and the roasting time was 3 h, the denitrification degree could reach 96.19%. When the mass ratio of sodium carbonate to aluminum dross was 0.8, the roasting temperature was 1000 °C, and the roasting time was 4 h, the denitrification degree could reach 91.32%. This study provides a reference for the non-harmful treatment of high nitrogen aluminum dross.