Following the June 1941 Axis invasion of the Soviet Union, Syrtlanova entered the military. Initially she continued to teach in Tbilisi, since the aeroclub became the 26th Military Aviation School of Pilots. After Axis forces made significant territorial gains and neared the Caucasus in September 1942, the school had to close. She then briefly served as a flight commander in a medical squadron in the Transcaucasian Front before joining the 588th Night Bomber Aviation Regiment in November. After arriving at the regiment in December 1942 she quickly gained a reputation as a confident, oriented, and successful pilot. Despite her relative lack of combat experience due to arriving at the front late, she eventually won promotion from pilot to flight commander, partially due to her vast amount of pre-war experience piloting the aircraft type used by the regiment, the Po-2. Not long after the unit was honored with a "Guards" designation and renamed as the 46th Guards Bomber Aviation Regiment in February 1943, Syrtlanova was awarded the Order of the Red Banner for completing 104 successful sorties. She continued tallying sorties throughout the war, completing 100 during the battle for the Taman peninsula (September-October 1943) and 172 in the battle for Crimea of April-May 1944, going so far as making eight sorties in one night, during one of which she took out an artillery battery. By the end of the war she had achieved the position of deputy squadron commander, and on 20 June 1945 she was nominated for the title Hero of the Soviet Union for having performed 780 sorties, dropped 104 tons of bombs on enemy territory, and safely guided her aircraft through heavy anti-aircraft fire and poor weather, destroying three artillery batteries, two searchlights, two trains, a fuel warehouse, and four ground vehicles. She was awarded the title on 15 May 1946.