Seasonal changes in the CO2 fixation rate and water-use efficiency in the leaves of six evergreen and two deciduous broad-leaved tree species on Jeju Island, Korea, were measured using a portable photosynthesis analyzer, to identify which species are most efficient in taking up CO2 from the air. The CO2 fixation rate was high in the deciduous species in spring and summer and decreased in fall, whereas it was high in the evergreen species in summer and fall and decreased in winter. The rate remained high in the deciduous tree Prunus yedoensis from spring to fall (> 7.1 μmol CO2/m2/s) and in two evergreen trees, Castanopsis cuspidata var. sieboldii and Cinnamomum camphora, in summer and fall (7.0 9.9 μmol CO2/m2/s). Therefore, these tree species fix atmospheric CO2 effectively. The water-use efficiency was higher in evergreen species than in deciduous species regardless of the season. Exceptionally, it was high in the deciduous species Zelkova serrata in spring and summer (> 100 μmol CO2/mol H2O), suggesting that Z. serrata is a useful tree for dry conditions due to its tolerance of water stress. The regressions of the CO2 fixation rate versus the evaporation rate and stomatal conductance were linear and non-linear, respectively. This suggests that the stomatal activity of leaves plays an important part in CO2 fixation of plants. In conclusion, C. cuspidata var. sieboldii, C. camphora, and P. yedoensis should be planted along roads or in urban spaces for the greening of cities and mitigation of CO2 concentrations in the air.