Cyanohydrins are valuable intermediates in organic synthesis. They enable an extensive chemistry that can be implemented starting either from the nitrile or from the hydroxy functionality. A number of challenges relevant to the enzyme-catalysed synthesis of chiral cyanohydrins have been addressed in recent years. In this review we will discuss three topics: (1) The enantioselective synthesis of cyanohydrins catalysed by Hydroxynitrile Lyases (Oxynitrilases); (2) The preparation of enantiopure cyanohydrins catalysed by hydrolases/ lipases via (dynamic) kinetic resolutions and (3) the (in situ) conversion of the enantiopure cyanohydrins, extending the use of cyanohydrins as building blocks in organic synthesis.