Cr-containing oxide pillared zirconium phosphate materials have been synthesized using the fluorocomplex method. They are active catalysts for the oxidation of ethane but present a low selectivity to ethene. In these materials the partial substitution of Cr cations by Ga or Al decreases the catalytic activity but increases the selectivity to ethene. The effect of the substitution of Cr3+ by Ga3+ or Al3+ on the selectivity to ethene during the oxidation of ethane can be related to the modification of both the oxidizing power and the acid strength of active sites. In this way, the higher the substitution of Cr the lower is both the oxidizing power of Cr cations and the acid strength of acid sites. The better selectivity to ethene was obtained on Ga/Cr-containing materials with a Ga/(Cr + Ga) atomic ratio of 0.4.