fabricable while we are facing increasing complexity in, for example, microelectronics. [6,7] For these reasons, challenges such as bad pattern alignment, [8,9] or pinch-off of pores and void formation [10][11][12][13] in top-down fabrication need to be addressed. On the other hand, a continuous film causes tradeoffs in desirable properties in many nanotechnological applications, such as losing mesoporosity while increasing the mechanical properties of an aerogel [14] or reducing catalytic activity while increasing catalyst stability against sintering. [15] To counter these problems, even atomic layer deposition (ALD), a method known for its superior conformality, has been expanded into area-selective fabrication by the addition of etching and functionalization steps in the workflow. [16][17][18][19] However, additional steps make the workflow increasingly slow, complex, and dependent on surface chemistries. There is also a growing interest in area-selectivity based on properties of precursors and substrates in ALD, [20] but new requirements on precursors would narrow down potential reagents. Furthermore, even conformal methods would leave voids inside ink-bottle-shaped pores and under composite undercuts [21] because conformal methods would clog the pore mouths before filling the internal parts. These problems have very recently revoked calls for profound changes and even a paradigm shift toward selective functionalization in the nanoscale. [18,20,[22][23][24][25] Special attention should be paid to inherently non-conformal methods, especially if they are surface-selective towards cavities. This includes both surface-selective subconformal coatings, those that coat only extremities and protrusions of a substrate, and surface-selective superconformal coatings, those that fill or coat cavities.Bottom-up approaches could eliminate the aforementioned problems while reducing the needed steps for surface-selective treatments-instead of breaking or carving things smaller and using miniaturized techniques (top-down), coatings could be grown self-aligning (bottom-up). One bottom-up category is surface-shape-selective deposition. Currently, this category has limited approaches, which are often based on either anisotropic processes such as directional plasma etching [26] or reagent flux, force fields, [27] competitive adsorption, [28] or reagents and additives with specific properties. [22] Truly bottom-up gap-filling technologies, especially those free of line-of-sight limitations, Nanotechnology drives technological progress in many frontiers, from electronics to medicine, from tougher composites to adaptive surfaces. As the feature sizes are made smaller, the importance of surfaces is increased. Many of the most powerful methods for surface manipulation are variants of vapor deposition (VD). However, VD is typically not surface-selective and, therefore, extra work steps are needed to integrate the methods into nanofabrication routines. Furthermore, many fields are moving toward 3D nanostructures, which unavoidably means...