3-Mercaptopropionic acid (3MPA) is a popular coating material for the preparation of aqueous quantum dots, yet its isomer 2-mercaptopropionic acid (2MPA) has not been much studied. Here, we present a detailed study on the aqueous synthesis of CdS quantum dots with a 2MPA coating. Reaction variables such as the Cd/S ratio, 2MPA/Cd ratio, pH, and temperature were individually studied to evaluate the influence of these variables on particle size and luminescence. At the optimum ratios and reaction conditions, a quantum yield (QY) as high as 54% was achieved. These quantum dots (QDs) have exhibited excellent colloidal and photostability over eight months of study. The color of the emission can be tuned by the reaction temperature and/or Cd/S ratio. 3MPA-coated CdS nanoparticles were prepared at various 3MPA/Cd ratios for comparison. The highest QY achieved for CdS−3MPA was 15%, and the luminescence decreased dramatically overtime. Ab initio calculations and spectroscopic characterization did not reveal a sign...