Nanoscience and nanotechnology have had great success in revealing nanostructures with unique dimensionalities. To highlight a few, nacre is composed of nanolayers of inorganic crystallites and biopolymers [1] and is therefore 2D in nature and exhibits extraordinary toughness. [2,3] Derivatives of such a structure can be utilized to suit a variety of engineering applications due to their fine structure. Nanotubes, nanobelts, or nanofibers all possess a 1D structure, where the long dimension promotes applications for advanced functional materials and the short dimension delivers superior electronic, mechanical, or electromechanical properties. Long-lasting impacts of these 1D features are being generated in multiple fields. For example, nanotubes could be used as scanning probes to provide unprecedented resolution to scanning probe microscopy, [4,5] continuous nanofibers can be efficient intermediate layers in nanocomposites, [6,7] and functional nanobelts demonstrating an electromechanical coupling effect can be potential candidates to power future nanosystems. [8][9][10] While nanoparticles or nanodots qualify as 0D structures and also have peculiar electronic or optoelectronic properties, their role as building blocks for higher-order subjects is one of their most prominent features. Demonstrated examples include packed particle films for high sensitivity detection, [11] fabricated arrays for photonic crystals, [12][13][14] and layered pores for energy storage. [15,16] More interestingly, it is even possible to form laminates of nanolayers with a carefully designed manufacturing and surface chemistry approach, rendering the formation of artificial nacre. [17,18] Properties of resulting assemblies usually exceed that of individual nanoparticles, where a large surface-to-volume ratio is believed to be one of the reasons for such a collective effect.With so much evidence for the structural flexibility of nanoparticles, stumbling blocks still impede the control of the growth of these 0D elements into a 1D assembly. Major barriers to unidirectional growth are difficulties to attenuate the robust interactions between nanoparticles and their isotropic shape. Patterned templates or surfaces could guide the growth of these building blocks. [19][20][21][22][23][24][25][26][27] An anisotropic surface treatment atop nanoparticles could regulate their assembly to a certain degree. [28,29] Free-standing strings of nanoparticles are rarely observed. A good strategy to devise a high throughput manufacturing of these assemblies with decent uniformity and a large aspect ratio has not been reported.We present our strategy in this communication to make unidirectionally grown and template-free, i.e., free-standing, 1D nanostructures by using uniform nanoparticles. We call this newly discovered structure a particle-fiber, implying the 0D nature of the building blocks. These string-like structures are grouped into forests after fabrication and have a few unique features, such as a high aspect ratio (length vs. diameter ! 2500), a uni...