The catalytic cracking of polyethylene has been studied over two natural clays and their pillared analogues with a view toward assessing their suitability in a process for recycling plastic waste to fuel. Although these clays were found to be less active than US-Y zeolite around 600 K, at slightly higher process temperatures, they were able to completely decompose polyethylene. Their yields to liquid products were around 70%, compared to less than 50% over US-Y zeolite. Moreover, the liquid products obtained over the clay catalysts were heavier. Both of these facts are attributed to the milder acidity of clays, as the very strong acidity characterizing zeolites leads to overcracking. Furthermore, this milder acidity leads to significantly lower occurrence of hydrogen-transfer secondary reactions compared to US-Y zeolite, and as a consequence, predominantly alkenes were the products over the clay catalysts. An additional advantage of these catalysts is the considerably lower amount of coke formed.