I wanted to learn Ancient Greek so that I could read Plato (well, Socrates, really) and Sappho, not so much for the aesthetics. I do like the iota subscript *, but I'm not too excited aesthectically about the rest.
I'm always wanted to learn Arabic, however, because of the incredible beauty of the calligraphy. I'm not really very interested in the literature (althrough I probably should be, as Baghdad was every bit as culturally important as Athens) but the writing is so damn pretty. Learning Arabic looks to be a lot of work, however.
Fortunately, there is a solution! C. C. Elian has painstakingly developed (over the course of the last twenty years) a sort of code for English that turns the normal letters into highly caligraphicable forms.
It's a pretty simple system, although you should read about it at her site. It's probably pretty easy to read, too. Once you've practiced a bit, I mean. And it looks really cool!
*I have no idea what that site is about, but it sure looks interesting. Better examples of the iota subscript may be seen here, along with a rough breathing mark and a circumflex. "Hey", with a rising and then falling pitch, I'm told: