AbstractColloidal quantum dots (CQDs) are emerging materials for short‐wave infrared (SWIR, ≈1100–3000 nm) photodetectors, which are technologically important for a broad array of applications. Unfortunately, the most developed SWIR CQD systems are Pb and Hg chalcogenides; their toxicity and regulated compositions limit their applications. InSb CQD system is a potential environmentally friendly alternative, whose bandgap in theory, is tunable via quantum confinement across the SWIR spectrum. However, InSb CQDs are difficult to exploit, due to their complex syntheses and uncommon reactive precursors, which greatly hinder their application and study. Here, a one‐pot synthesis strategy is reported using commercially available precursors to synthesize—under standard colloidal synthesis conditions—high‐quality, size‐tunable InSb CQDs. With this strategy, the large Bohr exciton radius of InSb can be exploited for tuning the bandgap of the CQDs over a wide range of wavelengths (≈1250–1860 nm) across the SWIR region. Furthermore, by changing the surface ligands of the CQDs from oleic acid (OA) to 1‐dodecanthiol (DDT), a ≈20‐fold lengthening in the excited‐state lifetime, efficient carrier multiplication, and slower carrier annihilation are observed. The work opens a wide range of SWIR applications to a promising class of Pb‐ and Hg‐free CQDs.