A Ni/Ce0.8Zr0.2O2 catalyst (NiCeZr-N) was synthesized by a facile co-nanocasting technique for syngas production from ethanol dry reforming. In addition, a series of characterization techniques, such as transmission electron microscopy (TEM), X-ray diffraction (XRD), inductive coupled plasma Emission Spectrometer (ICP), X-ray photoelectron spectroscopy (XPS), Raman and hydrogen temperature programmed reduction (H2-TPR) were selected to evaluate the physicochemical features of the as-prepared catalysts. Indeed, the results indicated that NiCeZr-N catalyst prepared by co-nanocasting method had a smaller particle size (<5 nm), relatively higher specific surface area (39m2/g) and stronger metal-support interaction in comparison with another model catalyst obtained from conventional co-precipitation method (NiCeZr-P). Expectedly, these positive factors enabled NiCeZr-N catalyst to exhibit better activity and stability. Typically, ethanol is completely converted by using NiCeZr-N as catalyst and heating to 700 °C, and CO2 conversion was as high as 65.3%. Interestingly, H2/CO was close to 1.1 at 650 °C, which could be used as feedstocks of Fischer-Tropsch process. Particularly, no obvious fluctuation of ethanol conversion and the product selectivity was observed during 40 h time-on-stream stability test.