Self-assembly, a fundamental process at all scales, [1] plays a vital role in nature and provides an important guidance for design and fabrication of functional materials. [2] Particularly, self-assembly provides an attractive and practical methodology for creating artificial nanostructures that promise broad impacts and applications in the emerging field of nanoscience. For example, self-assembled nanoparticles can lead to novel optical materials [3] and high-density magnetic recording media; [4] self-assembled monolayers [5] have enabled nanometer thickness organic films to be constructed on a variety of substrates for modeling biological surface to control the fate of cells, [6] building molecular electronic devices, [7] developing nanolithography, [8] and generating nanostructures for biomedical diagnostics; [9] and the self-assembly of oligopeptides [10,11] and other organic molecules [12] has resulted in nanofibers as the functional matrices of hydrogels that find possible applications in tissue engineering, [10,13] inhibitor screening, [14] and wound healing. [15] Although these works reflect the exciting and important development of self-assembled nanostructures in a non-biological arena or extracellular settings, intracellular creation of artificial nanostructures remains less explored and its subsequent biological effects largely unknown despite of its potential significances and applications.To explore intracellular artificial nanostructures is significant for several reasons. First, self-assembled nanostructures (e.g., cell membranes, strands of nucleic acids, actin filaments) prevail in living cells and are indispensable for critical cellular functions (e.g., as structural motifs for maintaining integrity of cells, as effective storages for keeping genetic information, and as active devices for regulating numerous cellular processes), therefore intracellular artificial nanostructures provide an attractive and effective strategy from perturbing the cellular activities to managing the behaviors of cells. Second, many diseases are related to mishaps in cellular nanostructures (e.g., mismatch of base pairs, formation of b-amyloid, and misfolding of proteins), hence intracellular artificial nanostructures offers a versatile and accessible platform for mimicking, modeling, and understanding the mechanism of diseases. Third, spectacular advances in molecular cell biology (i.e., the study of biological process at the molecular level) during the last five decades have led to new insights into the evolution of life forms, and now there is a need to correlate biological process beyond molecule level and to understand structure and dynamics as a system (i.e., system biology). Self-assembled intracellular artificial structures at the nanoscale lend a convenient means to examine the structure and dynamics of cellular functions and to allow previously unconnected domains of knowledge to be understood at new levels of complexity.Intracellular artificial nanostructures can result from different methodologies, ...