We report a successful one-pot synthesis of Cu-containing zeolites from Cu-tetraethylenepentamine complex Furthermore, these Cu-containing zeolites are employed as catalysts for evaluation for the dehydration of ethanol to ethylene, a typical model reaction for transforming bioethanol into valuable chemicals. Interestingly, these Cu-containing zeolites exhibit much higher catalytic performance than the corresponding zeolites and conventional catalysts for the dehydration of ethanol to ethylene. Particularly, these Cu-containing zeolites show very high low-temperature activity. For example, Cu-SSZ-13 zeolite achieved an ethylene yield higher than 99% at 212 degrees C. The introduction of the Cu species into zeolites offers an alternative way to develop highly efficient catalysts for the dehydration of ethanol to ethylene in the future.