This present disclosure provides methods for utilizing such forces in when generating nanofibrillar constructs with engineered morphology from the nano- to macro-scales. Using for example, a biopolymer silk fibroin as a base material, patterns an intermediate hydrogel were generated within a deformable mold. Subsequently, mechanical tension was introduced via either hydrogel contraction or mold deformation, and finally a material is reentrapped in this transformed shape via beta-sheet crystallization and critical point drying. Topdown engineered anchorages, cables, and shapes act in concert to mediate precision changes in nanofiber alignment/orientation and a macroscale form of provided nanofibrillar structure. An ability of this technique to engineer large gradients of nano- and micro-scale order, manipulate mechanical properties (such as plasticity and thermal transport), and the in-situ generation of 2D and 3D, multi-tiered and doped, nanofibrillar constructs was demonstrated.