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Core–shell CdSe/CdS nanocrystals are a very promising material for light emitting applications. Their solution‐phase synthesis is based on surface‐stabilizing ligands that make them soluble in organic solvents, like toluene or chloroform. However, solubility of these materials in water provides many advantages, such as additional process routes and easier handling. So far, solubilization of CdSe/CdS nanocrystals in water that avoids detrimental effects on the luminescent properties poses a major challenge. This work demonstrates how core–shell CdSe/CdS quantum dot‐in‐rods can be transferred into water using a ligand exchange method employing mercaptopropionic acid (MPA). Key to maintaining the light‐emitting properties is an enlarged CdS rod diameter, which prevents potential surface defects formed during the ligand exchange from affecting the photophysics of the dot‐in‐rods. Films made from water‐soluble dot‐in‐rods show amplified spontaneous emission (ASE) with a similar threshold (130 μJ/cm 2 ) as the pristine material (115 μJ/cm 2 ). To demonstrate feasibility for lasing applications, self‐assembled microlasers are fabricated via the “coffee‐ring effect” that display single‐mode operation and a very low threshold of ∼10 μJ/cm 2 . The performance of these microlasers is enhanced by the small size of MPA ligands, enabling a high packing density of the dot‐in‐rods.

Single‐Mode Lasing from Colloidal Water‐Soluble CdSe/CdS Quantum Dot‐in‐Rods