p-Xylene can be synthesized via a renewable route from biomass-derived 2,5-dimethylfuran (DMF) and ethylene with zeolite catalysts. Here, we propose mesoporous beta zeolite with a nanosponge-like morphology (NSP-BEA) as a highly efficient catalyst for the cycloaddition of DMF with ethylene. The NSP-BEA zeolite was synthesized through a hydrothermal synthesis route using multi-ammonium surfactants as a meso-micro dual structure-directing agent. From structural analyses and measurements of the surface acidity, the NSP-BEA was found to be composed of ultrathin zeolitic nanocrystals with intercrystalline mesopores (similar to 4.5 nm). It also possessed a large number of Bronsted acid sites on its external surfaces and in its internal micropores. This NSP-BEA catalyst exhibited high catalytic performance upon a cycloaddition of DMF with ethylene as compared to the commercial beta zeolite, alumina, and silica-alumina catalysts reported previously.