  Assembling nanostructured building blocks into network materials unlocks
macroscopic properties inaccessible with monolithic solids, notably toughness
and tolerance to electrochemical alloying. A method is reported for
large-scale, continuous synthesis of silicon nanowires (SiNWs) suspended in the
gas phase and their direct assembly into macroscopic sheets. Performing
gas-phase growth of SiNWs through floating catalyst chemical vapor deposition
using an aerosol of gold nanoparticles eliminates the need for substrates,
increasing the growth rate by a factor of 500, reaching 1.4 $\mu$m s$^{-1}$ and
leading to very long SiNWs. The combined high aspect ratio ($>$210) and large
concentration of SiNWs in the gas-phase (1.5 x 107 cm$^{-3}$) enable the
formation of macroscopic solids solely composed of percolated SiNWs, such as
free-standing sheets and continuous metre-long SiNW tapes. Sheet samples of
small diameter SiNWs ($<$25 nm) combine extraordinary flexibility in bending,
tensile ductility around 3%, and over 50-fold higher toughness than Si-based
anodes (fracture energy 0.18 $\pm$ 0.1 J g$^{-1}$). This synthesis and assembly
process should be applicable to virtually any one-dimensional inorganic
nanomaterial producible by thermochemical methods.
