I really have no help for you except to let you know that you are not alone. My Peanut (who is 16) has not pooped in the litterbox for many many many years. I've made sure they were cleaned regularly and even when they are sparkling clean and fresh, she still prefers the floor. The only consolation for me is that our litter boxes are in the basement (unfinished) so it doesn't matter if she poops on the floor. I just clean it up when I clean the litter boxes and it leaves no mark or smell - that I can smell anyway. However, I would be a bit more concerned if she was doing this in the living room like yours is.
You have two cats, have you got two litter boxes? "They say" that you should have at least one litter box per cat. I've got two cats and 3 litter boxes. Also, make sure they are clean and scooped, maybe he doesn't like using a dirty box? Or, like you say, it could just be behaviorial. Do you notice that he does this after you've been away for a few days? Or any other pattern you can think of, such as guests coming over or anything that could upset his normal routine might set him off.
Good luck and let us know how things go!
Tubby
Spring 1986 - Dec. 11, 2004
RIP Big Boy
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Peanut
Fall 1988 - Jan. 24, 2007
RIP Snotty Girl
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Robin
Fall 1997 - Oct. 6, 2012
RIP Sweet Monkeyhead Girl
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