A general, chemoenzymatic one‐pot procedure for the transformation of alcohols or amines to the corresponding alkene products in aqueous media has been reported. The procedure is based on the laccase‐TEMPO‐mediated oxidations of substrates and subsequent Wittig reaction. In this way, a one‐pot sequence of two consecutive reactions has been developed, which has a number of advantages such as (a) no need of purification of the intermediate products, (b) application of water as green solvent and an enzyme‐laccase as natural catalyst, (c) application of molecular oxygen as final green oxidant, and (d) formation of water as a byproduct of the oxidation step.