The Japanese paper arts origami and kirigami have revolutionized design of three-dimensional structures, metamaterials, and robots from planar materials. The design principles in these art forms are especially valuable for small systems because most nanofabrication involves lithographic patterning of planar substrates. In this thesis, we build upon efforts to bring these paper art forms to materials with a characteristic thickness on the scale of nanometers. We employ atomic layer deposition to synthesize films as thin as 2 nm and employ these films to create mechanical metamaterials, self-folding machines, and magnetic microbots. We begin this endeavor by developing fabrication methods to produce free-standing ALD films that are capable of integration with with complex nanofabrication processes. We employ these techniques to characterize the out-of-plane mechanical properties of ultra-thin films of inorganic metal oxides and metals. We build upon these results and fabricate mechanical metamaterials and magnetic mechanisms that exhibit emergent properties dictated by their geometries. In addition, we demonstrate that combinations of ALD materials form a versatile platform to achieve self-folding structures at the micron scale. Self-folding is then employed to produce electronically integrated robotics. Finally, we explore magnetically encoded microrobots, unifying the worlds of magnetic information storage and micromechanical systems.