A method of forming lightweight structures from particle networks includes functionalizing edges of particles of an anisotropic material, exfoliating of the particles to form sheets of the material, aligning the sheets of material to form a network of multi-layered and aligned particles, and forming a structure out of the network of particles. One example uses graphite powder mixed into 4-aminobenzoic acid for edge functionalization, and exfoliation occurs with sonication in a solvent. The resulting particles undergo alignment with an aligning nozzle that also dispenses the aligned particles to form a structure.