Mesoporous molecular sieve Zr‐MCM‐41 was modified with triethylenetetramine (TETA) and tested for carbon dioxide (CO2) adsorption for the first time. The adsorbent was characterized by powder X‐ray diffraction, N2 adsorption‐desorption, energy dispersive spectrometer, Fourier transform‐infrared spectroscopy, thermogravimetric analysis, and temperature‐programmed desorption of CO2 and NH3. A maximum CO2 adsorption capacity of 3.36 mmol g−1 at 50°C in a stream of 5% CO2 concentration was obtained, which is 2.7 times that of TETA‐functionalized MCM‐41. The TETA‐modified Zr‐MCM‐41 is 30°C higher than the TETA‐modified MCM‐41 in terms of thermal stability. We find that the former adsorbent is superior in reusability. It is envisaged that the adsorbent is applicable in CO2 capture. © 2015 American Institute of Chemical Engineers Environ Prog, 34: 1814–1821, 2015