A novel catalyst based on nickel supported on a folded sheet material (FSM) was synthesized and fully characterized. The resulting Ni-FSM-16 catalyst showed a high reactivity and selectivity in decarboxylation of plant-based carboxylic acids to yield the corresponding linear alkenes and alkanes in up to 75 % yield and less than 5 % of undesired cracking products. In addition, lignin-derived vanillic acid was smoothly converted to guaiacol. A comparative investigation showed that both the support and the metal of the Ni-FSM-16 catalyst proved to be pivotal for the reactivity. Particularly, substituting Ni with Fe, Pd or Al or replacing the FSM-16 support with MCM-41 or SBA-15 led to lower reactivity and selectivity towards linear decarboxylated products. The superior catalytic performance of Ni-FSM-16 was driven by a higher and more even metal distribution, more acidic silanol-group and an electron-rich, thus softer Ni, that promote coordination by the carbon-carbon double-bond of the fatty acid.