The Zr-pillaring of natural hectorite and synthetic laponite clay was investigated using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and thermogravimetric analysis (TGA) to characterize the different substrates. The difference in particle size of both clays is responsible for their differences in crystallinity, surface area (SA) and micropore volume (μPV) and consequently for their pillared forms too. Pre-adsorption of ethylenediamine in the interlayer space of laponite is performed in order to reduce the important contribution of edge-to-face and edge-to-edge stacking of the clay layers and creating a more homogeneous substrate for pillaring. As is proven by XRD, TGA and FTIR, ethylenediamine is exchanged completely for the Zr-pillaring precursors during the pillaring reaction. Surface areas and micropore volumes of, respectively, 482 m 2 /g and 0.34 cm 3 /g for Zr-pillared laponite and 171 m 2 /g and 0.064 cm 3 /g for Zr-pillared hectorite after calcination are obtained. Through pillaring, especially small pores (<0.71 nm), additional secondary micropores are formed with laponite while for hectorite, pores over a broad size range are observed. The prepared pillared interlayered clays (PILCs) were tested for their gas adsorption behaviour. Gas adsorption measurements on Zr-laponite reveal high adsorption capacities for N 2 and O 2 with a lowN 2 2 selectivity at 0°C.