Massive methane hydrates occur on sediment matrices in nature. Therefore, sediment-based methane hydrate systems play an essential role in the society and hydrate community, including energy resources, global climate changes, and geohazards. However, a fundamental understanding of mechanical properties of methane hydrate−mineral interface systems is largely limited due to insufficient experimental techniques. Herein, by using large-scale molecular simulations, we show that the mechanical properties of methane hydrate−mineral (silica, kaolinite, and Wyoming-type montmorillonite) interface systems are strongly dictated by the chemical components of sedimentary minerals that determine interfacial microstructures between methane hydrates and minerals. The tensile strengths of hydrate− mineral systems are found to decrease following the order of Wyoming-type montmorillonite-> silica-> kaolinite-based methane hydrate systems, all of which show a brittle failure at the interface between methane hydrates and minerals under tension. In contrast, upon compression, methane hydrates decompose into water and methane molecules, resulting from a large strain-induced mechanical instability. In particular, the failure of Wyoming-type montmorillonite-based methane hydrate systems under compression is characterized by a sudden decrease in the compressive stress at a strain of around 0.23, distinguishing it from those of silica-and kaolinite-based methane hydrate systems under compression. Our findings thus provide a molecular insight into the potential mechanisms of mechanical instability of gas hydrate-bearing sediment systems on Earth.