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I like Le Pain Quotiden in the ABC Carpet and Home building and The Adore (on 13th St, bet 5th and university place). LPQ is a very reliable chain with good open-faced sandwiches and large enough to accomodate more people. Tea drinkers will like The Adore's large selection, and the dining room is very toasty, quaint, smells deliciously of toasted bread and pastries, and perfect for small groups.
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We do the Greenmarket, EV Cheese, Whole Foods on Houston, Essex Street Market trek. So I'd probably walk to the LES and have breakfast at Shopsin's (check hours) or go to the Coffee Shop if there wasn't a line. My experiences at the Coffee Shop have been different from the other posters (I'm more in the Nikki NYC "okay" camp). To be fair, I have not been recently and there are better/cheaper places. There used to be an Ess-a-Bagel not far from Beth Israel. That's a short walk if you are a walker. No ambience, but good and inexpensive if you want carbs and nova. Meets OP request for casual, but I wouldn't consider it "fun."
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re: Nikki NYC
i'd say the food at Coffee Shop is several steps below ok...closer to "wretched".
i used to live in Union Square, and my fav breakfast place was Cafe Mogador, but that may be too far a walk (St. Marks between 1st/AveA) if you are toting a lot of Greenmarket produce. But thats where i'd go.
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