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Gas hydrate is considered as an emerging technique for natural gas storage and CH₄ separation from natural gas, because assorted nano-sized cages of gas hydrate allow selective trapping of specific gaseous guests such as CH₄, C₂H₆, and C₃H₈. When a mixture of CH₄, C₂H₆, and C₃H₈ forms gas hydrates with a liquid promoter at 5.6 mol%, sII large cages (sII-L) can be fully occupied by a promoter, while only CH₄ remains in the hydrate phase by occupying sII small cages (sII-S). Based on this, can CH₄ be selectively stored or separated from natural gas? Here, we aimed to elucidate the cage-filling behavior of gaseous and liquid guests in CH₄ + C₂H₆ + C₃H₈ hydrates formed with the addition of tetrahydrofuran (THF), trimethylene oxide (TMO), or 1,3-dioxolane (DIOX). We examined feasible strategies for synthesizing gas hydrate focusing on ice-borne or water-borne route. Our results suggested that ice …