A microscopic insight into hybrid CH₄ physisorption-hydrate formation in halloysite nanotubes (HNTs) is vital for understanding the solidification storage of natural gas in the HNTs and developing energy storage technology. Herein, large-scale microsecond classical molecular dynamics simulations are conducted to investigate CH₄ storage in the HNTs via the adsorption-hydration hybrid (AHH) method to reveal the effect of gas-water ratio. The simulation results indicate that the HNTs are excellent nanomaterials for CH₄ storage via the adsorption-hydration hybrid method. The CH₄ physisorption and hydrate formation inside and outside of the HNTs are profoundly influenced by the surface properties of the HNTs and the kinetic characteristics of CH₄/H₂O molecules. The outer surfaces of the HNTs exhibit relative hydrophobicity and adsorb CH₄ molecules to form nanobubbles. Moreover, CH₄ molecules adsorbed on the outer surface are tightly trapped between the hydrate solids and the outer surface, inhibiting their kinetic behavior and favoring CH₄ storage via physisorption. The inner surface of the HNTs exhibits extreme hydrophilicity and strongly adsorbs H₂O molecules; thus, CH₄ hydrate can form inside of the HNTs. It is more difficult for CH₄ and H₂O molecules inside of the HNTs to convert into hydrates than for those outside of the HNTs. A moderate gas-water ratio is advantageous for CH₄ physisorption and hydrate formation, whereas excessively high or low gas-water ratios are unfavorable for efficient CH₄ storage. These insights can help to develop an efficient CH₄ solidification storage technology.