Mussel byssus is a bundle of threads used to attach mussels to wet substrates. Recently, a thin cuticle layer on the byssus has attracted public attentions due to its remarkable toughness - stiff as epoxy resin and extensible as rubber. Here, we observed ultrastructure of the cuticle layer in a far eastern mussel (Mytilus coruscus) to understand underlying mechanisms for the mechanical properties. The cuticle layer observed by TEM was composed of submicron-sized granular inclusions in a continuous matrix phase. In addition, ultrastructural study in the presence of tertiary amine (Tetraethylammonium, TEA) showed an evidence that the cuticle is stabilized by cation-π interaction.