AbstractAs a result of the global demand for sustainable products, a suitable alternative to the resorcinol-formaldehyde aerogels, which are frequently used as precursors for carbon aerogels, is searched for. In this study, the replacement of petroleum-derived formaldehyde with a natural, biobased crosslinker, namely 5-(hydroxymethyl)furfural (5-HMF) is shown, and the synthesis of renewable, monolithic tannin aerogels is demonstrated. Compared to well-known tannin-formaldehyde aerogels, this green alternative shows lower reactivity of the crosslinker associated with lower gelation times as well as lower specific surface areas at the organic stage. Nonetheless, the morphologies and synthesis-structure relationships follow similar trends for both tannin-based aerogels, e.g., the pore size is influenced by the initial pH in the same manner. The turnover to carbon aerogels by a carbothermal treatment results in enhanced high-specific surface areas of the tannin-5-HMF-based carbon aerogels, which are similar and even slightly outperform those obtained from tannin-formaldehyde aerogels. This suggests that they are a convenient alternative for carbon aerogel applications. Graphical Abstract