<p>Complex organic molecules are of great importance to academic and industrial chemistry and typically synthesised from smaller building blocks by multistep reactions. The ability to perform multiple (distinct) transformations in a single reactor would greatly reduce the number of manipulations required for chemical manufacturing, and hence the development of multifunctional catalysts for such one-pot reactions is highly desirable. Here we report the synthesis of a novel hierarchically porous

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... ramework, in which the macropores are selectively functionalised with a SO₄/ZrO₂ solid acid coating, while the mesopores are selectively functionalised with MgO solid base nanoparticles. The spatially orthogonal distribution of acid and base catalytic sites permits the efficient two-step cascade deacetylation and Knoevenagel condensation of dimethyl acetals to cyanoates, and the simultaneous esterification and transesterification of a high free fatty acid content triglyceride.</p>