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My kids loved, mysteriously, Fritz Lang's Metropolis. Starting from ages 3 and 5 and continuing to today (going on 6 and 8). Metropolis is something they come back to again and again. I finally bought it after about six library checkouts and two lengthy visits via Netflix.
They also love old Fleisher Bros. cartoons (Betty Boop and Popeye).
And, not as old but pretending to be, Young Frankenstein is a much-loved favorite at our house.