- You can setup a TCP port to Smoothie from a Raspberry Pi but it's an annoying bit of work and you can't print from it that way (from the Pi, you can trigger an SD card print but then what's the point).
- You can connect by USB and it works. You can even print from USB but you'll probably run into performance problems at some point.
- I haven't tried using the UART.
Basically, I have an OctoPi setup and disconnected it because it was more of a pain than it was worth since I couldn't turn off my printer with the Pi attached (USB power) and printing from my LCD and SD card is easy enough.
Good luck and, definitely, let us know if you find more positive results!