. . . I wouldn't mind a 4:1 ratio compared to the current 2.7:1
Be careful what you wish for. I have a Rubicon with the NV241OR 4:1 transfer case. On many trails I found the low range ratio to be too low (i.e. engine rpm higher than my liking) and wished I had a 2.5-2.7:1 low range ratio for those situations.
Since I have a 42RLE automatic transmission I resolved the issue with a Rubi-Crawler so I now have 2.72:1, 4.0:1 and 10.88:1 low range ratios. Of those ratios I use 2.72:1 the most - by a wide margin. On a run Father's Day Weekend I didn't really need the 4.0:1 low range at all.
A rudimentary cost/benefit analysis suggests that unless you are into technical rock crawling you might be better off changing your 3.73 axle gear ratio to better suit your 33" tires and leaving your transfer case alone.
Food for thought.