I tried JustUnfollow.com, Tweepler.com , Friendorfollow.com, and Twitnest. Most of those solutions either did not work, or I simply didn't like the layout much. Not saying they are not goodies, but Refollow.com has to be the best solution to unfollow your users, and it does sooo much more.
Select User Criteria
The top select box controls who you see. If you want to search for people that you followed, but they didn't follow you, select the obvious choice of I'm Following mixed with Not Following Me. Voom, there you go.
User Display

After you choose your criteria you will see the users show up in the display area. Here you will see information about the users when you mouse over their avatar. This should help you make a decision about who to keep and who to boot.
Controls and Extras

The controls allow you to select multiple users and perform an action on them. You can unfollow, follow, block, lock, and unlock users. Lock and unlock are useful to keep those you want to follow even though they will not follow you back.
Now below these controls are some cool tools that allow you to quickly see who Mr. X is following or even who is following Mr. X. It works so gosh darn good you'll want to cry. Twitter has never been this easy.