In the last few years, the amidinium⋯carboxylate interaction has emerged as a powerful tool for the relatively predictable construction of families of three dimensional hydrogen bonded organic frameworks. These frameworks can be prepared in water and are surprisingly stable, including to heating in polar organic solvents and water. This feature article describes the design and synthesis of these materials, discusses their structures and stability, and highlights their recent applications for enzyme encapsulation and as precursors for the synthesis of molecularly thin hydrogen bonded 2D nanosheets.