Exploring sensing materials with superior catalytic properties is of paramount importance for acetone detection. In this work, NiO/NiFe₂O₄nanocubes derived from Ni/Fe bimetal metal-organic frameworks (MOFs) precursors are synthesized by one-step impregnation method and subsequent annealing process. The microstructure and morphology of the synthesized samples are investigated by a series of characterization. The results indicate that uniform and porous NiO/NiFe₂O₄nanocubes are formed. The gas sensing properties of NiO/NiFe₂O₄composites are systematically evaluated. Benefitting from the synergistic effect of abundant sites, p-p junction and high surface area, the optimal sensors based on NiO/NiFe₂O₄(Ni/Fe=1.5 at) exhibit the best sensing performance. The sensors show the highest response (19.9–100 pm acetone), short response/recovery times (2.4 s/19.6 s), low detection limit (200 ppb) and a good humidity tolerance ((S_{35% RH}-S_{95% RH})/S_{35% RH}= 0.095) to acetone at 200 °C. The results offer us a promising alternative to develop an ideal platform for acetone detection.