5‐(Hydroxymethyl)furfural (5‐HMF) is a vital platform molecule from which a variety of high‐value‐added fine chemicals and polymerizable monomers can be prepared. The use of solid acids to catalyze the conversion of biomass into 5‐HMF is environmentally friendly and economical. However, exploiting the high yield of 5‐HMF in a highly concentrated reactant system is challenging. Herein, we present a laser‐assisted method for preparing highly acidic monolithic acidic catalysts. A monolithic acidic catalyst based on metal Zr sheets was synthesized and used to catalytically convert 30 wt% fructose into 5‐HMF (conversion rate: 96%; yield: 95%). The catalyst was immediately separated from the reaction solution by direct removal at the end of the reaction. Catalytic efficiency was largely unaffected after 10 cycles of use, and the same catalytic efficiency was observed after laser‐regeneration, highlighting the potential industrial applicability of the developed catalyst.