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Precise control of structural parameters through nanoscale engineering to continuously tailor optical and electronic properties of functional nanomaterials remains an outstanding challenge. Previous work focused largely on chemical or physical interactions that occur under ambient pressures. In this article, we introduce a new pressure-directed assembly and fabrication method that uses a mechanical compressive force applied to nanoparticles (NPs) to induce structural phase transitions and consolidate new nanomaterials with precisely controlled structures and tunable properties. By manipulating NP coupling through external pressure instead of through chemistry, a reversible change in assembly structure and properties can be demonstrated. In addition, over a certain threshold, the external pressure forces these NPs into contact, allowing the formation and consolidation of one- to three-dimensional nanostructures. Through stress-induced NP assembly, unusual materials engineering and synthesis, in which morphology and architecture can be readily tuned to produce desired optical and electrical properties, appear feasible.