I think the store's officially called Anime Stop, and it's in the Bleeker Mall right next to The Comic Book Shoppe.
I think it's actually owned by the same people as the Comic Book Shoppe. I guess the anime/manga section inside The Comic Book Shoppe's Bleeker Mall location on Clyde/Merivale was getting so big that they decided to move their selection into a separate store proper.
As you can see from the mess of a sign above the store, that particular storefront is kind of a retail black hole, having been Dewar's Audio at one point, and then Silvio's Gifts. Let's hope Anime Stop will succeed where the two stores that were there before failed. (I did my part... I ordered the first volume of Barasui's Ichigo Mashimaro/Strawberry Marshmallow manga while I was there.)
They painted several anime characters in the window (clockwise from top right: Kyou Sohma from Fruits Basket in his cursed orange cat form, Edward Elric from Fullmetal Alchemist, Naruto Uzumaki from Naruto (duh), some guy who is either a generic anime-esque male character, some existing character whom I just don't recognize, or a really terrible drawing of Kyou Sohma in human form, and some generic, slightly lolicom, anime schoolgirl character.)