<p>Replacing fossil resources with cellulose presents a promising strategy to reduce dependence on and consumption of nonrenewable resources. Selective conversion of cellulose to levulinic acid (LeA) is one of the attractive depolymerization routes for producing a broad range of value-added chemicals, thereby offering opportunities to enhance both environmental sustainability and economic viability. To achieve high selectivity in LeA production, solid Pickering interfacial catalysts (PICs) were designed by embedding Brønsted (B) acidic/redox heteropolyacids (HPAs) H₅PMo₁₀V₂O₄₀ (HPMoV) inside the surface-functionalized ZrO₂ nanoparticles as HPMoV(n)@ZrO₂(C₈/C₅NH₂) (n represents loading amount of HPMoV, n = 15, 20, 25, 30 and 35 wt%, C₈ and C₅NH₂ represent C₈H₁₇ and C₅H₁₀(NH)NH₂). PIC HPMoV(30)@ZrO₂(C₈/C₅NH₂) exhibited notable catalytic activity in cellulose hydrolysis into LeA with 70.8% yield and 90.3% conversion at 120 ℃ for 7&#xa0;h. The enhancement of catalytic performance was attributed to several factors: stronger B acids combined with Lewis (L) dual sites ensured the breakage of β-1,4-glycosidic bonds and isomerization, which was a pivotal step for further transformation; the flexible surface of C₈ and C₅NH₂ in HPMoV(30)@ZrO₂(C₈/C₅NH₂) stabilized the water-in-oil (w/o) emulsion and concentrated the cellulose to accelerate its hydrolysis; simultaneously, the micro-ball milling effect induced by tough ZrO₂ nanoparticles further promoted rapid cellulose conversion. As a heterogeneous catalyst, PIC HPMoV(30)@ZrO₂(C₈/C₅NH₂) demonstrated exceptional longevity and stability, positioning it as a promising candidate for practical applications in cellulose conversion.</p> Graphical abstract <p></p>