I've had my CapsLock bound to Compose for ages; it's a great use of that piece of keyboard realestate.
I still don't have a good way to discover compose sequences other than by groveling through xkb and compose files. I really wish there were a character-palette tool that would tell me how to type the characters by introspecting the current input settings.
Why stop there though? Mine is configured to be ESC when tapped, CTRL when held down. Took a while to get used to, but it's a big improvement compared to other ways of handling ESC on a 60% keyboard.