The lubricating ability of graphite largely depends on the environmental humidity, essentially the amount of water in between its layers. In general, intercalated molecules in layered materials modify their extraordinary properties by interacting with the layers. To understand the interaction of intercalated water molecules with graphene layers, we performed Raman measurements on bi-layer graphene at various humidity levels and observed an additional peak close to that of the low-frequency layer breathing mode between two graphene layers. The additional peak is attributed to the vibration between an intercalated water layer and the graphene layers. We further propose that the monolayer coverage of water increases between bilayer graphene with increasing environmental humidity while the interaction between the water layer and graphene layers remains approximately unchanged, until too much water is intercalated to keep the monolayer structure, at just over 50% relative humidity. Notably, the results suggest that unexpectedly humidity could be an important factor affecting the properties of layered materials, as it significantly modifies the interlayer interaction.Graphite, the most prominent layered material, has been used as a good lubricant for about 200 years. However, an abnormally high wear rate of graphite brushes in electrical machines aboard aircraft during World War II was reported. 1 Later in the 1960s, NASA found that graphite lost its lubrication in space. 1 It is not the low pressure, but the low humidity, that is primarily responsible for the reduced lubricating ability at high altitude or in space, as a small amount of interlayer water is essential for the easy shear parallel to the graphene hexagonal planes. 2 A complete understanding of this has not been achieved as it is not yet clear how the interlayer water interacts with the graphene layers.Layered materials containing different numbers of layers can now be produced, either by exfoliating from the bulk, 3 or by stacking one layer onto another. 4 Structures made from different numbers of layers may possess unique properties. 5 Intercalated molecules further modify these properties. This vast research area focuses in general on three questions -how, and how many, intercalating molecules can be introduced between the layers, and what effect they have on pristine layered material. The properties of layered materials largely depend on their interlayer interaction. 6 It is therefore important to quantify the effect of intercalated molecules on this interaction.In our work we start with a simple system, bi-layer graphene (the simplest layered structure) with intercalated water (the most common polar molecule), while the amount of water is varied by adjusting the humidity (one of the most common atmospheric conditions).Much work has been done on water in between graphene oxide layers (GO), as it is hydrophilic -water easily comes between the layers and attaches to them via non-covalent bonds. 7 Early work reported interlayer spacings of 0.63 nm for dry...