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Three-dimensional (3D) hierarchical materials are important to a wide range of emerging technological applications. We report a method to synthesize complex 3D microengineered materials, such as microlattices, with nearly fully dense truss elements with a minimum diameter of approximately 20 μm and having high aspect ratios (up to 20:1) without using any templating or supporting materials. By varying the postprocessing conditions, we have also introduced an additional control over the internal porosity of the truss elements to demonstrate a hierarchical porous structure with an overall void size and feature size control of over five orders of magnitudes in length scale. The method uses direct printing of nanoparticle dispersions using the Aerosol Jet technology in 3D space without templating or supporting materials followed by binder removal and sintering. In addition to 3D microlattices, we have also demonstrated directly printed stretchable interconnects, spirals, and pillars. This assembly method could be implemented by a variety of microdroplet generation methods for fast and large-scale fabrication of the hierarchical materials for applications in tissue engineering, ultralight or multifunctional materials, microfluidics, and micro-optoelectronics.