I believe "Understanding Media" is his biggest one; source of his most famous quote "the medium is the message"
edit: There are also more polemic anti-tech presentations of his ideas, especially by Neil Postman or Nicholas Carr which are good in their own way. But to me the fascinating thing about McLuhan himself is his dedication to presenting his views in a such a matter-of-fact way that most of his early followers were probably very antithetical to his personal beliefs.