The last time I used a tool, excluding via robots.txt was also sufficient for URL removal.
Recently, Google has updated their documentation to strongly encourage you to use URL removal only for things like exposing confidential information, and not to clean up old pages or errors in your GWT account (see http://support.google.com/webmasters/bin/answer.py?hl=en&answer=1269119). I know many people still use the tool for that type of stuff, but wanted to point out that change.