Through a series of x-ray diffraction, optical spectroscopy diamond anvil cell experiments, combined with density functional theory calculations, we explore the dense CH4−H2 system. We find that pressures as low as 4.8 GPa can stabilize CH4(H2)2 and (CH4)2H2, with the latter exhibiting extreme hardening of the intramolecular vibrational mode of H2 units within the structure. On further compression, a unique structural composition, (CH4)3(H2)25, emerges. This novel structure holds a vast amount of molecular hydrogen and represents the first compound to surpass 50 wt % H2. These compounds, stabilized by nuclear quantum effects, persist over a broad pressure regime, exceeding 160 GPa.