Can I use the frame as the negative path in place of the battery to charger cable? Is this considered beneficial/safe/recommended/worth the effort ... etc, etc.?
Yes, you can and the frame will have less resistance in most cases. The downside is that you'll also have to establish a ground to frame from the battery. Also, you'll now have two additional ground connections. For most, that isn't an issue but for some purists it is additional failure point.
I'd suggest to just replace what you have with 4 ga welding cable and call it a day. I can buy good 4 ga for around $1/ft. I do my own terminations. If you don't crimp cables, you could pull the 6 ga, measure the lengths, and have Genuinedealz.com make new cables with terminations already prepared.