<P><B>Abstract</B></P><P>The enzymatic oxidative decarboxylation of linear short‐chain fatty acids (C4:0–C9:0) employing the P450 monooxygenase OleT, O<SUB>2</SUB> as the oxidant, and NAD(P)H as the electron donor gave the corresponding terminal C<SUB>3</SUB> to C<SUB>8</SUB> alkenes with product titers of up to 0.93 g L<SUP>−1</SUP> and TTNs of >2000. Key to this process was the construction of an efficient electron‐transfer chain employing putidaredoxin CamAB in combination with NAD(P)H recycling at the expense of glucose, formate, or phosphite. This system allows for the biocatalytic production of industrially important 1‐alkenes, such as propene and 1‐octene, from renewable resources for the first time.</P>