Heterogeneous catalysis is no longer restricted to the catalytic upgrading of recalcitrant lignin wastes from the pulping and paper industry. This discipline now offers innovative solutions for the lignocellulose deconstruction, generating “easy-to-upgrade” lignin streams along with cellulose pulps. In this issue of Joule, Beckham, Román-Leshkov, and colleagues report the first example of “tandem” lignin-first biorefining in which the formation and extraction of lignin oligomers in addition to the reductive processes leading to further depolymerization and passivation of lignin fragments are performed in two-sequential flow-through reactors. Heterogeneous catalysis is no longer restricted to the catalytic upgrading of recalcitrant lignin wastes from the pulping and paper industry. This discipline now offers innovative solutions for the lignocellulose deconstruction, generating “easy-to-upgrade” lignin streams along with cellulose pulps. In this issue of Joule, Beckham, Román-Leshkov, and colleauges report the first example of “tandem” lignin-first biorefining in which the formation and extraction of lignin oligomers in addition to the reductive processes leading to further depolymerization and passivation of lignin fragments are performed in two-sequential flow-through reactors.