Materials with three-dimensional (3D) hierarchical architectures exhibit attractive mechanical, energy conversion and thermal radiative cooling properties not found in their bulk counterparts. However, implementation of hierarchically structured 3D transition metal dichalcogenides (TMDs) is widely deemed not possible, by the lack of manufacturing solutions that overcome the hierarchy, quality, and scalability dilemma. Here we report dewetting-driven destabilization (DDD) process that enables simple, template-free, high throughput printing of 3D architected MoS2 Foam with hierarchy spanning seven orders of magnitude — from angstroms to centimeters. Although extremely simple, our manufacturing process combines electrohydrodynamic printing with dewetting-induced-patterning. This technique can be applied to a range of dissimilar twodimensional (2D) layered materials, including Ti3C2Tx MXene and reduced graphene oxide (rGO). The deposited MoS2 Foam achieves amplification of resilience and conductivity. It constructs hierarchically porous and spatially interconnected networks for both ions and electrons transfer. We further demonstrate the 3D MoS2 architected foam as high-performance anodes with an otherwise unachievable combination of a 99% battery yield, a dynamic recovery (up to 85%) to withstand excessive volume expansion, a strain-induced reduction in diffusion barrier (0.2 eV), and improved electron transport abilities across the entire structure. The result is the high Li-ion charge storage capacity with robust cycling stability at a bulk scale (~3.5 mg/cm2) and under a high current density (10,000 mA/g). The outstanding electrochemical performance arises from the architected structure-induced pseudocapacitive energy storage mechanism based on the redox reaction of Mo, rather than the traditional conversion reaction. Notably, the performance achieved is on par with or surpasses state-of-the-art anodes made of black phosphorus composites, Si-graphene and mesoporous graphene particle anodes, while the technique offers an evaporation-like simplicity for industrial scalability. This work is foundational, and the developed DDD process opens a new sight to manufacture structurally robust, multifunctional hierarchical structures from 2D materials. Given the high adjustability of synthesis conditions and a wide variety of 2D materials, we anticipate previously unattainable possibilities in the energy storage, flexible electronics, catalysis, separation and drug delivery.