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The stock 205 (or similar transfer case) has 4HI, 2HI, 4LO and neutral.
"Twin sticking" a transfer case allows you to have independent control of each shift rail (hence two shifters rather than one) which allows you to use front wheel drive only and 2LO.
This is especially useful for a "front dig". Generally you would set the rear line lock (or e-brake I suppose), put the t-case in front wheel drive and use just the front wheels to move the front of the truck to one side or the other. With a front dig you're not trying to make the obstacle just change the position of the truck. This can be especially useful in making tight turns too.
There is a good clip of a front dig at just over 2 minutes into this video.
And again this buggy makes a tight turn at the end of this video using a front dig.