When we went on a walking tour around Soho, our tour guide only had one recommendation when asked where to go for afternoon tea, and this place was it. You actually have to walk into a pub on the first floor called "Coach & Horses" and then ask to be let into the tea room. It is the cutest little place and all the pastries and jams are made in-house. You can go and have afternoon tea (which is what we did) or you can ask for a full menu and actually have lunch up there. I loved the atmosphere, the service, and the tea/pastries we ordered. If you are looking for the highly-stereotyped afternoon tea experience in England then this is your place.
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