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I've gotta go with The Wire. The Sopranos is a great show, but The Wire just seems more relevant, more real.
One thing I like about The Wire is how it reveals major plot twists with no fanfare, no string music, it just assumes that the viewer will get it, which adds to the realistic feel. For example, there is a certain extremely foulmouthed character who is a pain in the ass in the first two seasons. There is one quick wordless scene in Season 3, just a quick scan of a man in a place, that changes the entire way that we look at the character. No fanfare, no exposition, you either get it or you don't.
Also, the Wire never flinches while showing us how rotten the system is in a way I don't think we've ever seen on television before. In real life, intelligent caring professionals who know how to effect real positive change if allowed are instead forced to spend their time catering to the whims of their superiors, as seen with the pissing contest between Valchek and Sobotka in Season 2. This is contrasted with the cold blooded efficiency of the drug dealers, who play a real-life game of Risk with street corners and project buildings.
To put it in a nutshell, the Sopranos may be a bit more entertaining, but the Wire is a lot more important.