I'm a fan of Filicori.
Their coffee's good - try the lattes! I've had cold sugary drinks here, though my preference leans towards their hot offerings. Drink a lot of coffee? Ask about their bulk purchase option!
Haven't tried their baked goods.
The baristas I've encountered have are courteous and friendly, and somehow remember me even they've got no shortage of patrons. (They ARE right by the Charging Bull statue at Bowling Green.)
This is one of the tiniest Filicori locations, be aware.