It's a little moment, but in the song "Chu-Chi Face" when Baron Bomburst and the suit of armor snap their fingers in frustration at the same time. Of course the suit of armor isn't animate, but the laws of reality can be broken for a good gag, right?
Actually, the whole song itself is quite amusing.
I always loved the spies trying to be English with horribly out-of-date information as to how the locals really dressed and acted.
Not to mention their classically slapstick antics while trying to capture Caractacus and Chitty, including mistaking Grandpa Potts for the inventor — hilarious.
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