I've gotten alot better at driving tone where I'd like it since I first got my electric. However, I'm yet to find a use for using the "both pickups" feature of my les paul. When do you guys think that'd be a good idea? What kind of sound would I be going for.

I tend to use the neck pickup for bluesy leads and rhythm riffs and the bridge pickup for rockier stuff or to get that piercing feel to it. I guess my question is, why use both simultaneously?
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i thought that too, but heres what i do, it sounds pretty good, don't know how it will be with your rig but it sounded great with mine. I put treble on 10, 10. And then for rhythem i did .5 on volume, and 4.5 for tone, with my amps gain on 3, it sounded pretty nice, i use that set up alot now.
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I use the middle setting alot. It has more treble than the neck but still keeps some bass. I use middle for something like NIB for the main riff then to the neck for the slower heavy chord section.
On my Explorer, I use the middle setting the most, especially for playing rhythm. When playing stuff like A7X I leave it on the middle setting.
I tend to put one of the pickups' volume on 10 and the other at around 6 or so when I use the middle setting. I think it actually sounds pretty good.
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use a combination of your 2 volume knobs and tone knobs play around until you find a sound you like, generally that would be smoother on a clean channel.
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I hate the middle setting. It gives me really shitty Pinch Harmonics (Hardly audible). I get the strongest Harmonics off my neck pickup (EMG 81 in the neck, 85 in the bridge. If it's a passive pickup, it's usually a Bill Lawrence (The guy, not the company) in XL500L in the bridge and some sort of high gain pickup in the neck.)

I'm really diggin' the 81' 85' switch. I like the sound better than using the 81 in the bridge, and 85 in the neck.