the near future by constructing all-around NWs field-effect-transistors (NWFETs), complementary metal-oxide-semiconductor (CMOS) inverts, etc. [6,7] On the other hand, with narrow bandgaps of 0.35 and 0.77 eV, InAs and GaSb NWs are also considered as the ideal channel semiconductors for next-generation high-performance infrared photodetectors, demonstrating high responsivity of ≈10 4 AW -1 and detectivity of ≈10 12 Jones for near-infrared to middleinfrared at room temperature. [8][9][10] Especially, with a closing bandgap (1.42 eV) of Shockley-Queisser limit, typical III-V semiconductor of GaAs NW has been studied in the fields of not only infrared photodetectors but also high-efficiency solar cells. [11][12][13][14] Owing to the extreme photon collection boost in free-standing NWs, the efficiency of single GaAs NW can be as high as 40%. [14] Recently, for achieving high-performance broad-spectrum photodetectors, ternary alloy III-V semiconductors of InGaAs NWs and GaAsSb NWs with full composition range have become the research stars. [15][16][17][18][19] The hot development of wearable or flexible optoelectronic devices is challenging the research of III-V NWs. [20][21][22][23] Recently, lightweight structured fabrics with tunable mechanical properties enabled by non-convex interlocked particles have been realized by Wang et al. [20] Obviously, the successful growth of largescale high-quality III-V NWs on the expected novelty functional fabrics directly will promote the next-generation wearable or flexible electronics and photoelectronics. In the past decades, metal-organic chemical vapor deposition, molecular beam epitaxy, metal-organic vapor phase epitaxy, and chemical vapor deposition (CVD) methods are the commonly adopted technologies for the growth of high-quality III-V NWs. [24][25][26][27][28][29][30][31][32][33] Generally speaking, expensive wafers of GaSb, InAs, GaAs, InP, etc. are used as the growth substrates for overcoming the lattice mismatch during NWs growth process. [34,35] Fortunately, metals of Au, Sn, Pd, etc. can be deposited on the selected substrates as growth catalysts for III-V NWs, followed by vapor-liquidsolid (VLS) or vapor-solid-solid (VSS) growth mechanism. [36,37] Generally speaking, during the VLS growth process, the adopted metals catalysts are liquid, which requires the eutectic Large-scale growth of high-quality III-V nanowires (NWs) on an expected substrate is challenging the next-generation optoelectronic devices. In this work, high-quality III-V NWs of binary GaSb, GaAs and ternary GaAs x Sb 1−x , In x Ga 1−x As are successfully prepared on the hard substrates of SiO 2 /Si, amorphous glass and flexible substrates of mica, glass fiber, and carbon cloth by adopting the simple and low-cost metal-catalyzed chemical vapor deposition (CVD) method. The homogeneity of morphology, crystallinity, and stoichiometry is checked by scanning electron microscopy, X-ray diffraction, high-resolution transmission electron microscopy, and energy dispersive X-ray spectroscopy, implying the high-q...