Smooth Operations is cool, but it's short. You'd be much better off getting Totally Out of Control, which is long, and awesome. There is just not enough material to make it worth your while (when you're just starting out). And as far as the Card College 4 goes, that's really a judgement call, it's not really about what tricks you know, but about what sleights you know. Because by volume four, they don't tell you what a top palm, classic pass, or automatic-turn-over is. You can risk getting it and not knowing what half the stuff is, or you can gradually work your way up.
Again I'd highly recommend TOOC, the rest is up to you,
Hope this helps,
-PTG