What a huge question!
I would start by saying that one mans "nicest control harmonisation" could well be another man's "bag of bolts". As you point out achieving good handling qualities across a wide envelope is more difficult than over a narrow one. This is where modern flight control systems really start to pay dividends. By this I'm talking about flight controls where the "gains" are variable depending upon whereabouts in the envelope you are and indeed what task you are undertaking. Phantom/Lightning/Harrier etc had gearing to change control response or control travel based on gear being up or down and to some extent depending on Mach number. But the likes of Typhoon has a variable schedule based on all of the above and in addition mass and cg location (long and lat). Advances in filght simulation now allow a great deal of refinement to be done in advance of flight test, but the proof of the pudding still (thankfully) comes from flying in the real air.
Tarnished
Edited to add more here:
http://www.pprune.org/forums/showthread.php?t=188151