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Due to the promising storage capacity for CH₄, the method of natural gas storage and transportation using solid gas hydrate is recognized as an alternative to conventional liquefied natural gas process. To make this alternative more viable, however, it is necessary to further shift the formation temperature and pressure of natural gas hydrate closer to ambient conditions. Although there is a trade-off between storing more CH₄ and mitigating the formation conditions, it is known that adding specific liquid molecules such as tetrahydrofuran, as a secondary guest to CH₄ hydrate could lead to favorable thermodynamic stability while still affording promising CH₄ storage capacity via a mechanism known as the tuning phenomenon. Here, this study focused on trimethylene oxide (TMO) + CH₄ hydrate to reveal its unique guest occupation patterns for potential application to natural gas storage and transportation. The …