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A synthetic ligand\/transition\u2010metal moiety is anchored covalently or non\u2010covalently to a host protein, thereby generating a single artificial metalloenzyme which can then be optimized by molecular biological methods. In the quest to construct an appropriate experimental platform for asymmetric Diels\u2013Alder reactions amenable to this Darwinian approach to catalysis, specifically those not currently possible using traditional chiral transition\u2010metal catalysts, two strategies have been developed which are reviewed here. One concerns the supramolecular anchoring of a Cu(II)\u2010phthalocyanine complex to serum albumins; the other is based on the design of a Cu(II)\u2010specific binding site in a thermostable protein host (tHisF), leading to 46\u201398%<jats:italic>ee<\/jats:italic>in a model Diels\u2013Alder reaction. 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