I prefer a pretty loose arrangement. Generally
Good = They're nice, most of the time.
Evil = They're a jerk, most of the time.
Lawful = They generally do what is expected of them by some sort of external social order or internal code of behavior.
Chaotic = They generally do whatever they feel like doing.
Well it isn't about alignment as in "What makes an alignment" this is about what makes a decent character that can be run in a setting.
A totally immoral character with no real connections, liabilities, or anything... Is a psychopath.
Sure Order of the Stick had Balker and he was "evil", but he was a kind of evil that could be directed and he definitely had some morals or inklings not to go around killing random people.
People just want to play the game's secret villain... but if they want to be the secret villain then just ask me if they can be the secret villain.
Not to nitpick, but the only things I remember doing that were threats of violence and magical compulsions.
But yes, a very large part of the time the people who want to play CE characters are the sort that think it would be absolutely hilarious to ape Belkar or Black Mage in a real campaign. So complete tools, in other words. LE isn't objectionable.
CN is sort of a borderline case. It's a really useful alignment for characters who are chaotic and not particularly nice (Rogues and Barbarians come to mind in particular), but it's also the alignment of choice for the tools who've been banned from playing CE.