Ba-ETS-4 is a promising adsorbent for nitrogen removal from low-grade natural gas. However, the Ba-ETS-4 adsorption characteristics, i.e., both adsorption kinetics and equilibrium capacity, change by dehydration temperature owing to structural shrinkage and pore contraction which finally impact the separation performance of the adsorption bed. In this paper, experimental breakthrough data are provided for N2/CH4 separation at various Ba-ETS-4 dehydration temperatures (250°C-450 °C) followed by a separation performance analysis in generating methane as the main product. Additionally, isotherm data at different temperatures (20 °C, 40 °C, 60 °C and 80 °C) are presented for selected dehydration temperatures (250 °C, 350 °C, 400 °C and 440 °C). The results revealed that an increase in dehydration temperature leads to a decrease in adsorption capacity but a better separation by providing more hindrance for CH4 diffusion, while not affecting the N2 breakthrough wavefront. At a dehydration temperature of 250 °C, theN2 breakthrough time is the highest, indicating the ability to process a larger feed. However, this also leads to the least CH4 production (0.037 mmol/g), as most of the fed CH4 is adsorbed onto the bed. Interestingly, an increase in dehydration temperature leads to an increase in CH4 production up to 420 °C (0.140 mmol/g), after which the CH4 production decreases sharply.