JAE,
Depending on your definition of 'largest', it either was definitively the largest, or quite likely the largest.
Since there is only a handful of taller structures than the WTC, by virtue of it being the only one that big to be demolished, it must be the largest. Therefore, a definitive 'yes' by that measurement.
If 'largest' is defined in terms of weight, I would guess that it is still the largest. After all, there aren't many structures in the world that can accomodate that many people; and the last opportunity for truly large-scale destruction was WWII, and there were even fewer structures of that size then. Of course, as soon as I make strong statement to this effect, I expect somebody will come along and prove me wrong.
One thing that I have thought about since the attacks--I wonder whether somebody is evaluating an approach similar to this as an efficient improvement to implosion of very tall structures. By no means am I intending to lighten the gravity of the situation; but as a naturally curious individual, it seems like structural engineers may be able to learn from the relative efficiency of this 'demolition'.
When I saw that coming down the first time, I initially presumed that the terrorists had somehow managed to wire it for an implosion, since it looked like a picture-perfect implosion of a building. How practical would local collapse, followed by dynamic crushing be? Or is this essentially what is already done?
As implosion is by no means my field, I'm curious if somebody else who knows more could comment on my line of thought.
Brad