There isn't that much anime in Harajuku, but there are plenty of other shops to look at.
To get there, you can take a JR train on the Yamanote line there. I can't remember which exit is the correct one, but it is a small station and a little exploration will get you on track. There is a road running parralel to the railway line. Opposite one of the exits is another road, usually full of people. There are also many people from shops shouting at you to go and buy something. Somewhere half way along this road is another road which goes up a hill. Not far along that is a Totoro shop. you can't miss it as there is a large stuffed Totoro outside. A little further in a basement level shop, some anime items can be found. Mainly Sailor Moon and Sanrio stuff.
Kamakura is quite far to the south of Tokyo. To get there take a train on the Yokosuka Line (dark blue). It may be faster to take a train on the Tokaido line to Ofuna and change there to the other line for the final part of the journey.
At Kamakura, the is only one anime shop, a Totoro shop near the station by other shops. With the help of a guide book, you can also explore the many temples in the area. There is also a beach with surf.
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