AbstractEnergy and dipole moment calculations show 3‐nitro‐5‐ amino‐1,2,4‐triazole is the most stable tautomer of ANTA either in the gas phase and polar solvents, in agreement with X‐ray findings. Our calculations predict that the 5‐nitro‐3‐amino‐1,2,4‐triazole tautomer is more sensitive to shock or impact. Some discrepancies between semiempirical (AMI and PM3) calculations and ab initio (up to 6‐3