I can't seem to figure out how to get that nice, sketchy look in GIMP.
'nough said?

Yup. Or pencil, or whatever people usually line art with.

People usually line art with the pen tool. I have a tablet, so I don't like to use it. But that's what people do :p
I like to download brushes from sites like deviantart, instead of changing around the settings myself. It's better imo.
http://browse.deviantart.com/resources/applications/gimpbrushes/?qh=§ion=&q= Try looking around?