When an atomically thin 2D material is suspended as a membrane so that adsorbed atoms can stick to both sides, these atoms can interact through the membrane and thus act as two coupled adsorbate systems, with new properties that are absent in either system alone. Computational modeling in the 2D Crystal Consortium predicts new patterns that emerge, such as an infinite staircase of fractional coverages of opposing sides with simple rational fractions being favored, a so-called “Devil’s Staircase.” Since adsorbate patterns are possible at different spatial scales, it is possible to obtain parallel staircases with different step heights, and even come arbitrarily close to violating a revered principle of thermodynamics, the Gibbs Phase Rule. These systems provide a new window into the behavior of atoms on surfaces.