Cafe Ladro is one of the few organic coffee places I've found in the city.  I used to frequent the downtown location because it was just a couple blocks from my office.  Today I hit the one on Capitol Hill.  There are both consistently good.
The coffee at Ladro is good.  The baristas are funky and friendly.  The pastries are good (downtown they have a carrot cake cupcake that is fantastic).  
Wi-fi is not free, but the nice folks at the store today offered to give me the credentials to bypass the payment (I declined).  I suspect this is SOP.
                        
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