Every neighborhood should have a coffee shop like Jack's Stir-Brewed Coffee, which serves only organic, fairtrade coffee, an incredible chocolate chip cookie, plus lots of tea, juice, and other treats. If it was just a smidge bigger, it'd have Central Perk potential, but I still love stopping by to meet a friend or read the Sunday Times. You can easily eavesdrop on conversations as you pretend to be engrossed in the Metropolitan section.
I met my brother here a couple days ago and we split one of Aunt Rosie's famous, perfect-sized chocolate chip cookies after a walk. Absolutely worth a stop if you're in the West Village!