LAUSR

Climate change and the depletion of fossil fuels increase the demand for sustainable energy. Biodiesel synthesized using heterogeneous acid catalysts is a promising clean‐energy carrier that supports a circular carbon economy. Herein, the efficient synthesis of biodiesel is reported using a reusable solid acid graphene catalyst functionalized with a natural aminosulfonic acid. Experimental and theoretical studies reveal the key role of functionalities that simultaneously contain amino and sulfonate groups, which impart superior acidity. Excellent activity and selectivity for oleic acid conversion to oleic acid methyl esters (a sustainable biofuel) are obtained, offering a strategy for achieving improved catalytic performance compared to earlier or benchmark catalysts in the field. Notably, the catalyst also effectively converts common vegetable oils into biodiesel via transesterification and facilitates carbohydrate dehydration to value‐added chemicals, demonstrating broad applicability. Two additional variants of aminosulfonic acid‐functionalized graphene show similar activity, confirming the crucial role of these functionalities in achieving high acidity and catalytic performance. The development of such potent, recyclable catalysts is crucial because acid catalysis is highly versatile, underpinning many biological and synthetic transformations.