Second for Taronga Zoo, but I'd suggest the Roar 'n' Snore - you stay in a tent (with a timber floor & power) overlooking the Harbour Bridge and do a night & morning safari. We did it at Christmas (my surprise gift to the family) and the kids loved it. The giraffes were my personal favorite.
Looks a bit pricey at first, but when you take into account the fact that it includes accommodation for 4 and 2 meals, it is actually quite reasonable.
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