The exceptional intrinsic properties of aligned nanofibers, such as carbon nanotubes (CNTs), and their ability to be easily densified by capillary forces motivates their use as shape-engineerable materials. While a variety of self-assembled CNT structures, such as cell networks, micropillars, and pins have previously been fabricated via the capillary-mediated densification of patterned CNT arrays, predicting the critical pattern size (s cr) that separates cell versus pin formation and the corresponding process-morphology scaling relations within the micrometer range are outstanding. Here, facile and scalable mechanical patterning and capillary densification techniques are used to establish s cr by elucidating how the effective elastic modulus of aligned CNT arrays during densification governs the resulting pin geometries. Experiments and modeling show that this effective modulus scales with CNT height and is about an order of magnitude smaller for pins as compared to cell networks formed from bulk-scale (i.e. non-patterned) CNT arrays. Patterning therefore results in pins with a lower packing density (commensurate with double the wall thickness) and a larger characteristic length scale than bulk cell networks (i.e. s cr ∼ 5 × cell width). CNT arrays with the initial randomly-oriented carbon 'crust' removed via oxygen plasma etching yield a higher degree of structural uniformity and better agreement with the proposed elasto-capillary model, which enables the use of capillary densification to predictively design hierarchical and shapetunable materials for advanced thermal, electronic, and biomedical devices. RECEIVED