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Lignin is a recalcitrant polymer arising from addition polymerization of phenylpropanoid units via an oxidative, enzyme-catalyzed radical mechanism. Lignin removal is a serious technological challenge in wood-related industries such as pulping for paper production. In this review, some outstanding aspects in lignin biosynthesis and structure are depicted; also the commonly used industrial protocols for pulp delignification are described, with special emphasis on their molecular aspects. A discussion is presented concerning the known chemical mechanisms of enzyme-catalyzed delignification by white-rot fungi. Biomimetic and bioinspired synthetic metalloporphines show monooxygenase/peroxygenase-like catalytic activity, being quite more versatile catalysts than ligninolytic enzymes (being capable only of one-electron oxidations). The advantages of this behavior are encompassed with an in-depth discussion …