γ‐Valerolactone (GVL) is a renowned starting material in production of bio‐fuels, valuable chemicals and polymers. The one‐pot tandem synthesis of GVL from furfural without a cumbersome intermediate separation/purification process is highly desired, yet the transformation remains challenging owing to the complicated reaction routes. Zirconium phosphate (ZrPO), a cheap and easily prepared solid catalyst with Lewis–Brønsted dual acidity, is herein discovered to enable one‐pot tandem transformation of furfural into GVL with using 2‐propanol as H‐donor/solvent to proceed smoothly. In addition, ZrPO prepared by hydrothermal method exhibits superior catalytic performance in comparison with the counterpart prepared by co‐precipitation method, giving a 42.7% yield of GVL at 180 °C. The difference in catalytic activity between ZrPO materials prepared by hydrothermal method and co‐precipitation method is linked with their morphology and acid sites density. Furthermore, the as‐prepared ZrPO catalyst works in a heterogeneous manner and can be reused for multiple times without significant deactivation. © 2022 Society of Chemical Industry and John Wiley & Sons, Ltd [ABSTRACT FROM AUTHOR]