Growth of high-quality single-crystalline InSb layers remains challenging in material science. Such layered InSb materials are highly desired for searching for and manipulation of Majorana fermions in solid state, a fundamental research task in physics today, and for development of novel high-speed nanoelectronic and infrared optoelectronic devices. Here we report on a new route towards growth of single-crystalline, layered InSb materials. We demonstrate the successful growth of free-standing, two-dimensional InSb nanosheets on one-dimensional InAs nanowires by molecular-beam epitaxy. The grown InSb nanosheets are pure zinc-blende single crystals. The length and width of the InSb nanosheets are up to several micrometers and the thickness is down to ~10 nm. The InSb nanosheets show a clear ambipolar behavior and a high electron mobility. Our work will open up new technology routes towards the development of InSb-based devices for applications in nanoelectronics, optoelectronics and quantum electronics, and for study of fundamental physical phenomena.*To whom correspondence should be addressed. E-mail: jhzhao@red.semi.ac.cn (J.H.Z.); hqxu@pku.edu.cn (H.Q.X.)Over the past several decades, the inherent scaling limitations of Si electron devices have fuelled the exploration of alternative semiconductors, with high carrier mobility, to further enhance device performance [1][2][3] . In particular, high mobility III-V compound semiconductors have been actively studied 4,5 . As a technologically important III-V semiconductor, InSb is the most desired material system for applications in high-speed, low-power electronics and infrared optoelectronics owing to its highest electron mobility and narrowest bandgap among all the III-V semiconductors. Recently, epitaxially grown InSb nanostructures have been widely anticipated to have potential applications in spintronics, topological quantum computing, and detection and manipulation of Majorana fermions, due to small effective mass, strong spin-orbit interaction and giant g factor in InSb [6][7][8][9][10][11][12][13][14][15][16][17][18] . All these applications require a high degree of InSb growth control on its morphology and especially crystal quality 19,20 . Unfortunately, due to the intrinsic largest lattice parameter of InSb among all the III-V semiconductors, epitaxial growth of InSb layers faces an inevitable difficulty in finding a lattice-matched substrate. Conventionally, buffer layers with graded or abrupt composition profile are deposited on lattice mismatched substrates to obtain a layer with a required value of lattice constant 21,22 . Nevertheless, even when the sophisticated buffer-layer engineering is used, the density of dislocations threading to the surface of the buffer from its interface with a lattice mismatched substrate is often too high to grow a high crystal quality InSb layer for fabrication of high-performance nanoelectronics and quantum devices and for study of novel physical phenomena.Here, we report on the successful growth of novel free-standing...