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For zeolite catalysts, the regulation of active site and pore structure plays an important role in the enhancement of their catalytic performance. In this work, a one‐pot and organic template‐free co‐regulation route is proposed to straightforwardly synthesize basic mesoporous ZSM‐5 zeolites with adjustable alkaline‐earth metal species. The synthesis pathway combines two decisive strategies: 1) the seed‐induced interface assembly growth method and 2) the acidic co‐hydrolysis/condensation of aluminosilicate species and alkaline‐earth metal (e.g. Mg, Ca, Sr, or Ba) sources. It is interesting that the mesoporous structure was self‐evolved through particle‐attached seed‐interfacial crystallization without the assistance of any template. Meanwhile, the incorporation of alkaline‐earth metals species is homogeneous and highly dispersed in the solid products during the whole crystallization process, and finally generate the superior basicity. Catalysis tests of the as‐synthesized samples displayed their novel performance in the typical base reaction of Knoevenagel condensation, even for bulky substrates owing to the enhanced diffusion arising from the meso/microporous network. This finding opens new possibilities for facile, cost‐effective, and environmentally friendly synthesis of mesoporous high‐silica zeolites with tunable acid/base properties, and deepens our understanding of the particle‐attached crystallization. [ABSTRACT FROM AUTHOR]