[4] On September 24–25, 1938, flying as pilot-in-command with Marina Raskova as navigator and Polina Osipenko as co-pilot, she completed the 5,910-kilometer-long flight named Rodina (Russian for "Motherland") on an Tupolev ANT-37, setting an international women's record for a straight-line distance flight (FAI Record File Number 10444).

In May, she was appointed the first commanding officer of the 101st Long-Range Aviation Regiment, which consisted of about 300 men: pilots, navigators, engineers and ground support personnel.

Her unit was equipped with Lisunov Li-2 transport aircraft (license-built versions of the Douglas DC-3) with pilots conscripted from the Civil Air Fleet.

The unit had initially the task of bombing enemy troops, to fly to partisans and – in June 1942 – to help supply the besieged Leningrad.

Subsequently, the 101st Long-Range Bomber Air Regiment was ordered to bomb Wehrmacht units that had broken the Bryansk and South-Western Fronts and were heading for Voronezh.

On Grizodubova's initiative, by March 1943 partisans had built an improved airstrip on the right bank of the Dnieper, where up to a dozen aircraft could be parked in daytime.

[8] In the 1940s she served as the sole female member of the "Extraordinary State Commission for Ascertaining and Investigating Crimes Perpetrated by the German-Fascist Invaders and their Accomplices" (Chrezvychainaia gosudarstvennaia komissiia or Чрезвычайная Государственная Комиссия; ChGK),[9] appointed to investigate Nazi war crimes in the Soviet Union and to compensate the state for damages.