Keep in mind the 6.2's seem to operate most efficiently at around 1800 rpm. lugging the motor lower than that can actually hurt fuel economy. A quick search online for "rpm calculator" will allow you to check gearing, tire size, and transmission ratio's to hit the sweet spot.
http://www.csgnetwork.com/multirpmcalc.html
example: with a TH400, 31 in tires, and 3.08 gears, going 65mph, should be turning the motor at 2170 rpm. swapping to the .70 overdrive in the 700R4 would put that rpm down to 1519.
for the record, the other danger of turning the engine that slow with the 700R4 is that IIRC you loose line pressure at lower rpms, causing slippage, increased operating temp, and premature wear of the clutch packs.
upping the speed to 80mph would put you in the sweet spot at 1869 rpm. putting 33in tires on there would drop that rpm to 1756. But with both, the 80mph headwind would most likely offset your increased operating efficiency.
with 31 in tires, 3.73 gears and the 700R4, youd cruse at 65mph at 1839rpm. this is the route i would go for a daily driver, and fuel economy. (although id do an NV3500 over the 700R4 personally). the smaller the tires, the less mass to spin, the less work the engine does, the less fuel it needs to burn. the deeper axle gears and deeper first gear of the 700R4 would make off the line acceleration dramatically better (more than double the gear ratio you currently have). and the combination would net easy high mileage highway crusing.