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From Book-Off's website, it seems there's no longer a shop in Harajuku.
The one in Shibuya on Centergai street looks pretty big... I've never been in it though. Check out the map here.
To get there from Hachiko exit, Shibuya station:
Cross the intersection, take the street on the left side of Starbucks (look up, there’s a large HMV sign).
Go straight past Sakuraya electronics shop (on the right).
Pass the following: