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Developing a highly active, acid-resistant and low-cost catalyst which can perform well in aqueous solution has long been sought for practical and sustainable lignocellulosic biomass transformation. In this work, a series of Ce–P–Co heterogeneous catalysts were prepared by a convenient solvothermal method for catalytic hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL) in water. By comprehensive characterizations and catalytic measurements, the structure of the prepared Ce–P–Co samples was disclosed as (CePO4)m/Co2P composites with a modulated molar ratio (m) of 0.04–0.34. With the introduction of CePO4, the unique hydrogen activation on CePO4 markedly accelerated the reaction, with the GVL yield after 90 min on (CePO4)m/Co2P (45–97%) being much higher than on pure Co2P (26%), together with an attractive TOF of 0.27–0.61 s−1 on (CePO4)m/Co2P (comparable to precious metal catalysts). Further analysis of the kinetic and acidic features indicated a Langmuir–Hinshelwood mechanism, initiated by activation of H2 and LA on CePO4 and Co2P, respectively, followed by a surface reaction of the two activated species as the rate-determining step, as a plausible pathway for producing GVL from LA on (CePO4)m/Co2P. The consistent catalytic performance during recycling tests and the unchanged morphological, bulk and surface structure features of the used catalyst relative to the fresh catalyst confirmed that the (CePO4)m/Co2P structure was robust enough to endure the acidic aqueous environment for efficiently and sustainably converting LA to GVL. The advantages of high catalytic efficiency, stable, acid-resistant structure and low cost marked (CePO4)m/Co2P as a competitive and practical heterogeneous catalyst for sustainable, scaled-up lignocellulosic biomass transformation. [ABSTRACT FROM AUTHOR]