To identify the origin of the magneto-LC effects, which refer to the enhancement of intermolecular magnetic interactions in the LC phases of all-organic radical compounds, we have designed and synthesized H-bonded all-organic radical compounds showing nematic and cholesteric phases for the first time. They show stronger magneto-LC effects than in the same LC phases of analogous covalent-bonded all-organic radical LC compounds. Variable-temperature electron paramagnetic resonance spectroscopy of the hydrogen-bonded compounds reveals that the inhomogeneous intermolecular contacts give rise to the magneto-LC effects.