One embodiment includes a nuclear magnetic resonance (NMR) gyroscope system. The system includes a vapor cell that encloses an alkali metal and a gyromagnetic isotope. The system also includes a magnetic field source that generates a magnetic field aligned with a sensitive axis of the NMR gyroscope system and which is provided through the vapor cell to cause the alkali metal and the gyromagnetic isotope to precess. The system also includes a laser that generates an optical beam that polarizes the alkali metal in the vapor cell to facilitate the precession of the alkali metal and the gyromagnetic isotope. The system further includes an angular rotation sensor configured to calculate a rotation angle about the sensitive axis based on a measured characteristic of a detection beam corresponding to the optical beam exiting the vapor cell, the characteristic being associated with the precession of the gyromagnetic isotope.