* Learn C. I have heard good things about _Learn C The Hard Way_, which is free, though I have never used it myself. Since you want to know more "CS," work through _Introduction to Algorithms_, a pretty standard (second-semester) university text, in C (NOT a language than manages memory for you!).
http://c.learncodethehardway.org/
http://mitpress.mit.edu/books/introduction-algorithms
* Work through _The Elements of Computing Systems_ (aka "From NAND to Tetris"). The book is fun, and it introduces many topics that are more advanced than CRUD.
I have many other ideas, but I decided to stop here in order to emphasize those above. :)