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In all its forms, catalysis accounts for 80% of all chemical processes worldwide, with biocatalysis playing a major part, as a 'white biotechnological' tool in sustainable industrial production. Biocatalysis complements the traditional chemical synthetic methods and offers a distinct approach to the synthesis of high-value chiral molecules. Chiral amine units are highly common in both the pharmaceutical and agrochemical industries. Biocatalytic strategies for the synthesis of chiral amines rely heavily on the use of ω-transaminases, enzymes impeded by their thermodynamic limitations in the synthetic direction, amongst others. This thesis describes an attractive alternative strategy to both the equilibrium-shifting problem and the low-cost availability amine donor, by employing biogenic polyamines, which are ubiquitous in all types of living cells. Moreover, they can be used in biomimetic enzymatic cascades for the synthesis of simple heterocyclic scaffolds of more complex alkaloids. The present thesis shows the research carried out as part of this PhD and it is formatted as a series of manuscripts, part of which have either been published or recently accepted for publication, together with a manuscript which is planned to be submitted to a peer-review journal in the near future.