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In this chapter, we describe electro-organic synthesis using a boron-doped diamond (BDD) electrode. First, a brief introduction about electro-organic synthesis is provided. This section begins with an explanation of a basic concept in electro-organic synthesis, followed by an introduction of the important milestones. Second, we focus on the electrochemical molecular conversions where the BDD electrodes play a significant role. This section begins with a review of electrochemical properties of BDD, followed by an introduction of reported examples such as anodic methoxylation and dehydrogenative anodic C−C coupling reactions. Third, we describe our approaches toward natural product synthesis via electro-organic synthesis using a BDD electrode: (1) anodic oxidation of the phenol compound possessing a phenylpropanoid framework and (2) cathodic reduction of aromatic carbonyl compounds.