* These two authors contribute equally to this work 2 Two paramount challenges in carbon nanotube research are achieving chiralitycontrolled synthesis and understanding chirality-dependent device physics 1-7 . Highthroughput and in-situ chirality and electronic structural characterization of individual carbon nanotubes is crucial for addressing these challenges. Optical imaging and spectroscopy has unparalleled throughput and specificity 8-14 , but its realization for single nanotubes on substrates or in devices has long been an outstanding challenge.Here we demonstrate video-rate imaging and in-situ spectroscopy of individual carbon nanotubes on various substrates and in functional devices using a novel high-contrast polarization-based optical microscopy. Our technique enables the complete chirality profiling of hundreds of as-grown carbon nanotubes. In addition, we in-situ monitor nanotube electronic structure in active field-effect devices, and observe that high-order nanotube optical resonances are dramatically broadened by electrostatic doping. This unexpected behaviour points to strong interband electron-electron scattering processes that can dominate ultrafast dynamics of excited states in carbon nanotubes.3 Single-walled carbon nanotubes (SWNTs) comprise a large family of tubular carbon structures characterized by different chiral indices (n, m), each having distinct electronic structure and physical properties 1 . They are promising materials for next generation nanoelectronic and nano-photonic devices, including field-effect transistors, light emitters and photocurrent/photovoltaics device [1][2][3][4][5][6][7] . Currently nanotube research faces two outstanding challenges: (1) achieving chirality-controlled nanotube growth and (2) understanding chirality-dependent nanotube device physics. Addressing these challenges requires, respectively, high-throughput determination of nanotube chirality distribution on growth substrates and in-situ characterization of nanotube electronic structure in operating devices.Direct optical imaging and spectroscopy is well suited for these goals [8][9][10][11][12][13][14] , but its realization for single nanotubes on substrates or in devices has been an outstanding challenge due to small nanotube signal and unavoidable environment background. Here we demonstrate for the first time high-throughput real-time optical imaging and broadband spectroscopy of individual nanotubes in devices using a polarization-based microscopy combined with supercontinuum laser illumination. Our technique is generally applicable to semiconducting and metallic nanotubes in various configurations, such as on (transparent or opaque) substrates, between contact electrodes, and under top gates. This is in contrast to strong constraints limiting other prevailing single-tube spectroscopy techniques: single-tube fluorescence spectroscopy only works for isolated semiconducting nanotubes 8 ; Rayleigh scattering requires nanotubes suspended or oil-immersed on transparent substrate 9-12 ; and resonant Ra...