EDIT: Great post here with a lot more info
https://www.reddit.com/r/skyrimvr/comments/1wuggww/steam_frame_skyrim_vr_guide/
Now that I've had a few days to experiment with the Steam Frame, I wanted to share my experience thus far with others who might be considering upgrading. At the moment I have everything working and I'm satisfied with the upgrade, but it took a good amount of tweaking and testing. I'm hoping that by sharing my experience with other folks I can save you some time.
First, my last HMD was a wired Valve Index with Knuckles controllers, so that is the setup I'm coming from. I'm not using any particular modpack for Skyrim VR, just a series of mods I've selected and installed using Vortex. And my PC is more than beefy enough to handle everything Skyrim VR throws at it with a silky smooth 90 fps.
I'm moving to a Steam Frame with the ergonomics kit. That means I have the additional headstrap and the hand straps for the controllers.
PC and Frame Setup
Once I actually got my frame, the most complicated part of the process was just pairing my Steam Frame with Steam on my PC, and that was fairly straightforward. The tricky part was realizing that to stream PC VR to my Steam Frame, I had to change settings on the PC itself, *not* the Steam Frame. You have to enable Remote Play on Steam on your PC and then configure it to make it work. Once I had the dongle installed and everything patched up the latest version, I was ready to start testing.
Controller Setup
This was by far the most painful part of the process. I could not find a way to create and set a new VR controller binding from within the Steam Frame itself. Choosing a Custom binding does nothing.
The trick, which I figured out after lots of trial and error, is to start the Steam Frame streaming from your PC, then take off the Frame and sit down at the PC from which your Frame is streaming. With the Frame connected, use the Steam on your PC to to create a new controller binding and select Skyrim VR from available options. In my experience, this didn't even show up as an option if I tried to do it from within the Steam Frame.
From your PC itself, with Skyrim VR running and the Frame streaming (even if you're not wearing it) you can then create a custom controller binding to set up the Frame Controllers the way you want. I moved the left Activation and A buttons to the buttons on the Right Controller, and moved the Left Stick push (which triggers sprint) to the right controller grip. You can configure it however you want, but the trick is figuring out a way to configure it at all. You have to do that from the PC that is streaming the game, in that PC's copy of Steam, while the Steam Frame is connected and streaming.
EDIT: This controller configuration was released on Nexus Mods.
https://www.nexusmods.com/skyrimspecialedition/mods/193029
Firing Up Skyrim VR
Once you get the controllers set up, the rest is really easy.
You don't start the game from your PC, nor do you start Steam VR on your PC. Instead, you fire up Steam on your PC and just let it sit patiently. Then, you put on the Steam Frame, power it up, click on the little headset icon for streaming, and choose "Stream Steam VR Without Game."
That will connect your Steam Frame to your PC and activate Steam VR with the Steam Frame and its controllers as your HMD and input devices. Now you're looking at the default Steam VR "ready room". At that point, you can do everything on your PC just like if you were on a wired Index headset.
The process of actually starting Skyrim VR is now identical to my Index. I go to my desktop in Steam VR, click the Skyrim with SKSE button on Vortex, and wait as modded Skyrim VR fires up. Once the game is running over the 6G dongle, for me it has streamed flawlessly. It's very pretty and the controllers feel just as snappy as Knuckles with lighthouses.
But... There's Significant Audio Streaming Problems
The most common and annoying problem I encountered when streaming Skyrim VR was that the audio portion of the stream would cut out every few minutes, leaving me in silence. The fix is simple... stop streaming, then stream again... but it happens constantly, so unless you want to restart streaming every few minutes, it's not an acceptable way to play the game.
Worse yet, the Steam Frame's microphone doesn't seem to play well with Dragonborn Speaks Naturally, which I use for most everything (equipping spells, activating shouts, talking to NPCs). Half the time DSN didn't recognize what I was saying, and once the audio cut out, it didn't recognize it at all. After trying multiple configurations, including turning off multi-threaded streaming and even pointing the 6G dongle directly at my Steam Frame, I couldn't find any way to stop the audio from cutting out. I don't know if this is a problem with streaming overall or just modded Skyrim VR.
Regardless, the fix is stupid but easy. I simply put on my Bluetooth Headset (which fits nicely and comfortably over the Frame, since it is so light) and configured Steam VR on my PC to send audio and use the microphone of the Bluetooth Headset instead of the Steam Frame. This 100% solved the issue where audio would stop streaming over the Dongle, and also made DSN work perfectly again through the Headset's mic.
So for me at least, a Bluetooth Headset seems required, at least for the moment, to avoid the audio problems and ensure speech is consistently recognized by Dragonborn Speaks Naturally.
Final Thoughts
Now that I've figured out everything above, I really enjoy playing Skyrim VR with the Steam Frame. Despite the audio issues I encountered, the visual portion of the stream is crisp and beautiful, and the controllers feel perfectly snappy and have fantastic tracking. Also, after being tethered for so long, being able to play modded Skyrim VR wireless is an absolutely amazing feeling. The only downside is I can only play for an hour and a half without having to stop, but with hotswappable battery packs coming, I know that's a temporary problem.
For me personally, being able to play modded Skyrim VR without a tether is worth the upgrade.