Interference lithography (IL) is an elegant fabrication technique that allows the creation of 1D, 2D, and 3D periodic patterns and predetermined highly porous architectures. [1,2] This technique enables easy control over pattern geometry via the means of changing the wavelength and angles between the beams. [3,4] IL is promising for fast microfabrication of complex 2D and 3D surface films unachievable by other techniques and, more importantly, it facilitates top down, one-shot synthesis of bicontinuous open structures in conformal multifunctional polymer coatings. IL enables submicrometer-sized elements (nodes and beams) with complex 2D and 3D lattices with micrometer to submicrometer spacings. [5][6][7] Turberfield and co-workers were the first to demonstrate the transfer of a 3D holographic interference pattern into a polymer photoresist.[8] The resulting structure was reminiscent of an interconnected diamond network. It was the first convincing experimental demonstration that large-area 3D structures could be fabricated on the submicrometer-size scale with low defect densities. Thomas and co-workers and Yang and coworkers demonstrated a variety of IL structures from elastomers with easily deformed architecture. [9,10] However, to date, these periodic structures have been primarily pursued for photonic and phononic applications. [11][12][13] On the other hand, for a variety of demanding applications, the design key is to select appropriate polymeric materials for creating the ''skeleton'' structures with good mechanical properties and appropriate geometry and symmetry for proper mechanical load distribution.[14] The understanding of elastic and plastic behavior and the ultimate fracture behavior of the IL structures and corresponding organized microcomposites, all become paramount criteria. Apart from the unique mechanical applications, nanoparticle-decorated porous structures can also be highly advantageous in catalysis, flow-through reactions, filtration, and microfluidic and sensing applications. [15,16] Creation of such sophisticated multicomponent microcomposites with bicontinuous organized architectures has not yet been achieved. Particularly, the ability to fabricate reinforced organized structures can be critical in light of recent results, which demonstrated collapse of such structures under compressive stresses. [17][18][19][20] Moreover, traditional reinforcing approaches, such as adding an inorganic component (e.g., metal nanoparticles) to the precursor or adsorbing them onto fabricated structures, are not readily applicable because of interference with photopolymerization, capillary-induced collapse, and clogging of nanoscale pores. We have previously demonstrated organized bicomponent IL polymeric microstructures by infiltration of a rubbery component (such as polybutadiene and polyacrylic acid) into a SU8 microframe.[21] While the bicomponent polymeric structures exhibited excellent mechanical properties under tensile stress with the rubbery component bridging cracks in the SU8 matrix, they are r...