They can indeed, but the can't do it spontaneously. There has to be a case to base it on. This may provide the basis for such a case.
Madison had slipped away from his Nationalist beginnings by 1829 and his original belief that the states were a positive detrement to National development and should be eliminated. The Constitutional Convention was called as much for economic reasons as political according to many.
That may be, but his observatsion on the original intent of the Commerce Clause remain, and help establish the basis for determining that Congress' use of the Commerce Clause has indeed exceed the authority granted to it by the representatives of the States that transferred that power.
That is all well and good. But the main issue is whether a state can nullify a federal law. It cannot.
I believe the state could have challenged this law in court without the grandstanding.