Nuclear Magnetic Resonance (NMR) is a powerful spectroscopic technique with a variety of applications in chemistry, biochemistry, materials science, and medicine. Conventional NMR, often referred to as 'high-field NMR', leverages the interaction between nuclear spins and a strong external magnetic field. In this technique, nuclei resonate at frequencies uniquely determined by their type and the surrounding chemical environment, offering detailed insights into molecular structure and dynamics. Conversely, in ZULF NMR, intrinsic interactions within molecules are stronger than couplings of nuclei to the applied external magnetic field. ZULF NMR offers several benefits over conventional high-field NMR. One key advantage is its reliance on internal spin interactions, such as J-couplings, rather than the external magnetic field, allowing access to untruncated spin Hamiltonians, thus, offering unique spectroscopic insights. 11 Additionally, ZULF NMR avoids line broadening due to insensitivity to susceptibility-induced gradients from the sample, enabling high-resolution spectroscopy even for inhomogeneous samples. The technique also benefits from reduced equipment complexity, cost, and improved portability, as it does not require strong magnets. Furthermore, the low-frequency signals in ZULF NMR can penetrate conductive materials, allowing measurements in otherwise challenging environments, e.g., some industrial applications. Conventional NMR generates detectable signals by utilizing thermal polarization of the sample achieved in strong magnetic fields. In the context of ZULF NMR, this approach involves temporarily applying a higher field to the sample before performing detection or shuttling the sample from high field to ZULF. However, even after thermalization at high fields, nuclear signals are often still insufficiently strong. To address this limitation, hyperpolarization techniques are employed; they generate spin polarizations that significantly exceed thermal levels, thereby producing much larger signals. Among these techniques, SABRE is particularly notable for producing hyperpolarization directly at low fields, enabling in situ detection. Furthermore, SABRE allows for initialization of specific spin orders which makes its combination with ZULF NMR a particularly versatile platform for generic ensemble nuclear spin-order control. The SABRE method uses singlet spin order of parahydrogen (pH 2 ) to prepare hyperpolarization on a molecule of interest (in this work, acetonitrile ) that undergoes reversible exchange with Ir-based organometallic complexes in solution, Fig. ). These complexes act as polarization-transfer catalysts (PTCs), facilitating the transfer of spin order from pH 2 to substrate molecules bound to the complex. Through multiple exchange events, the transferred spin order accumulates on the free substrate molecules in solution.