This paper investigates the dynamical properties of the spin‐coupling ensemble, with a focus on the spin‐decoupling phenomenon. The nuclear spin in such systems is significantly impacted by the electron spin when the main magnetic field approaches the Fermi contact field of nuclear spin, leading to measurement inaccuracies. A comprehensive dynamics model of the electron‐nuclear spin coupling ensemble has been established and analyzed. It proposes that the primary magnetic field augmenting effectively disentangles the precession frequency of the two spin‐coupling species, thereby yielding a spin‐decoupled state. Such a state allows nuclear spin serves as a high sensitive element for magnetic field measurements, while electron spin serves as a probe to acquire the precession of nuclear spin. With proposed method, a magnetic field resolution of 0.75 nT in a 12000 nT environment is achieved, indicating potential for magnetic field detection in geomagnetic environments. It further demonstrates measurements of electron spin Fermi contact interaction and polarization based on spin‐decoupling and in situ nuclear spin precession, results indicate measurement errors close to 1%. These results demonstrate the effectiveness of our approach in improving the accuracy and sensitivity of magnetic field measurements in spin‐coupled systems such as co‐magnetometers, nuclear magnetic resonance gyroscopes, and nuclear magnetometers.