As an atheist Jillette sees all religious people as crazy. He's right to point out that Pelosi, as an apparently real believing Catholic, is just as crazy as Palin if being religious makes you crazy. To look down on Palin for her religiosity while not looking down on Pelosi is therefore, in Jillette's view, inconsistent. But this reaction to Palin versus Pelosi isn't surprising because if Palin supported positions of the Left and was religious then her religious beliefs would be either forgiven or celebrated for how they support the Left's agenda.
Here's Nancy expressing the depth of her belief in the same religion that Sarah embraces.
His rant is about how when Rand Paul argued for a right to free association in the private sphere the Left attacked him for not being more sensitive to what the populace wants to hear. Of course, the Left was really attacking Paul for saying things that they do not want the populace to hear. Unqualified support for right of free association is an idea that works against the goals of the Left.
Update: I'd like to note that I do not see religious people as any crazier than the bulk of the rest of the population. I find certainty about the God stuff among some atheists to be tedious and irrational. Atheists can't prove God does not exist. Atheists can't explain why reality exists at all (and I can't either). There are things beyond our ability to understand and a certain amount of humility is called for.
While I'm at it: I find the term "crazy" is overused. Lots of people are wrong, deluded, ignorant, too stupid to understand key topics of public policy, or any combination of the above. But that does not make them crazy. It just makes wrong or deluded or ignorant or dumb or some combination thereof.
Certainly lots of people (including people who make to to the Oval Office) are so irresponsible about how they form and promote their beliefs that they are dangerous. But, again, that does not make them crazy. It just makes them dangerous and irresponsible.
A lot of looking down at religious people amounts to claims of higher status. "Oh look at those crazy religious people. I am so superior." More often than not the committed secularist who strikes such poses has embraced deluded secular beliefs that are a greater threat to the commonwealth than the religious views he's deriding. As someone points out in the comments, Penn Jillette sounds just plain crazy about immigration (total open borders). Well, Jillette isn't really crazy. But he's irrational and irresponsible, kinda like Sarah Palin and Nancy Pelosi.