Al or Ti oligo-cations were added to aq. 1% Na-form montmorillonite (Mt) (9.4% Fe2O3) to achieve the Al(or Ti)/mont-morillonite ratio10 mM/g. The montmorillonite was dried 12 h/393 K, ion-exchanged (24 h, 333 K) with aq. Fe3+, Cu2+ or Co2+ (as nitrates), redried, calcined 12 h/673 K, degassed in He 0.5 h/673 K and tested as catalyst in the reduction of NO with NH3, or C2H4 in a (0.25:0.25:2.5:97 v/v) NO-NH3 (or C2H4)-O-2-He reaction mixture, 40 mL/min, over 373743 K. With Mt-Al-Fe and Mt-Ti-Cu, NO conversions were 100% over 530-670 K (at >670 K, 02 oxidized NH3) and 540-640 K, resp.. Mt-Al-Cu converted 100% NO above 670 K. Mt-Ti-Fe converted 50% NO at 750 K. Oxide pillars increased the interlayer distance from 0.32 (Mt-Na) to 0.87 nm, and thus also the sp. surface (from 38 to 85-286 m(2)/g) and microporosity (from 35 to 48-76%).