One of most unique and fascinating features of natural biomineralization processes is the controlled growth and hierarchical organization of inorganic minerals along with organic materials. Such marvels of nature give excellent physicochemical properties to natural biomaterials [1][2][3] and provide inspiration for the synthesis of novel functional nanomaterials to chemists and materials scientists. [4][5][6][7][8][9] For example, natural bones with excellent mechanical properties are a kind of organic/inorganic hybrid materials with organic collagen nanofi brils and inorganic calcium phosphate nanocrystals hierarchically organized on a nanoscale. [ 10 ] Researchers have found that the hierarchical organization of organic and inorganic components of natural biomaterials is due mainly to the repetitive display of acidic functional groups on the surface of organic materials [ 2 , 11 ] that can act as a nucleation site for the growth of inorganic materials. In this regard, numerous efforts have been made to synthesize novel hybrid nanomaterials by mimicking biomineralization processes especially for biomedical applications. [12][13][14][15] For example, Hartgerink and colleagues reported on synthesis and mineralization of peptideamphiphile nanofi bers displaying phosphate groups on their surface for bone regeneration. [ 13 ] To date, however, the synthesis of industrially important hybrid nanomaterials by mimicking biomineralization processes has been rarely reported despite many potential advantages of biomimetic approaches such as environmental compatibility and high controllability of shape and size.On the other hand, interest is growing in the fabrication of functional nanomaterials by self-assembly of peptide-based building blocks because of functional fl exibility and environmental compatibility. [ 16 , 17 ] Among numerous self-assembling peptides reported to date, diphenylalanine (Phe-Phe, FF) and its derivatives [18][19][20][21][22][23][24][25][26][27][28][29][30] are simplest peptides exhibiting unique mechanical, [ 19 ] electrochemical, [ 20 ] and optical properties [ 21 ] as well as high thermal and chemical stabilities. [ 23 ] It has been reported that they can readily form various nanostructures, including nanotubes, [18][19][20][21][22] nanowires, [23][24][25][26][27] nanospheres, [ 28 ] organogels, [ 29 ] and hydrogels [ 30 ] through a self-assembly process. Here, we fi rst report the synthesis of transition metal phosphate nanotubes for application as a cathode material for rechargeable lithium (Li) ion batteries by using a peptide hydrogel self-assembled from fl uorenylmethoxycarbonyl (Fmoc)-FF [ 30 ] as a template. The peptide hydrogel is composed of very thin nanofi bers (diameter about a few tens of nm) and displays numerous acidic and polar moieties on its surface (Figures S1 and S2 in the Supporting Information), which are highly benefi cial for the synthesis of novel organic/inorganic hybrid nanomaterials.We synthesized peptide/transition metal phosphate core/ shell nanofi bers, as schematic...