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We experimentally demonstrated that composites, being effective in optimizing the thermoelectric performance, can also enhance photothermoelectric effects in this work. In detail, we employed an alternating-growth in chemical-vapor-transport to grow the SnSe–SnSe2 composite crystals. The photo-responsivities of SnSe–SnSe2 (atomic-weight-ratio as 44%–56%) composite are comparable to SnSe crystals in the visible band (444 and 532 nm). However, the responsivities of SnSe–SnSe2 have remarkable 27.3% enhancement than those of SnSe crystal at the near-infrared band (1310 and 1550 nm). Supported by optical spectroscopy and theoretical electronic band structure, the enhanced optical responsivity of SnSe–SnSe2 composites is due to the formation of P–N junctions at interfaces between SnSe and SnSe2, leading to more optical transition channels and corresponding optical absorptions in near-infrared band. Our work verifies that hetero-junction formed among constituent compounds in composites is effective in optimizing the photothermoelectric response of thermoelectric materials in certain electromagnetic bands, paving the way to develop photoelectric detection devices. [ABSTRACT FROM AUTHOR]