The selective oxidation of tetrahydrofuran (THF) to gamma-butyrolactone (GBL) on spinel ZnFe2O4 nanoparticles (ZFNPs) was investigated. The catalyst was prepared with the coprecipitation method and characterized by FTIR, XRD, TEM, SEM, EDS, TGA, XPS, and BET surface area. The characterization techniques showed that a nonuniform spherical spinal oxide with an average particle size of 26 nm was formed. The oxidation reaction was carried out using hydrogen peroxide as an oxidizing agent under solvent-free conditions. GC-MS analysis revealed that the main product was GBL. 2-hydroxytetrahydrofuran (THF-2-OH), gamma-hydroxybutyric acid (GHBA), and gamma-hydroxybutaldehyde (GHBAl) were obtained as minor products. The effects of different reaction parameters, such as temperature, H2O2/THF mole ratio, catalyst dose, reaction time, and reusability, were evaluated. A 47.3% conversion of THF with an 88.2% selectivity of GBL was achieved by conducting the reaction at 80 °C for nine hours using a 1:1 mole ratio of H2O2/THF. A slight increase in the conversion degree was attained at higher temperatures; however, an over-oxidation process was observed as the temperature exceeded 80 °C. The catalyst remained effective and stable over four reuses.