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should I block this IP?
It has to be your choice entirely. Only you know the content of your site and it's visitors patterns.
If you only had 100 visitors in a month that 35% might just be somebody interested in your sites.
If you had 1000 and upwards than 35% is a substantial number.
What ever this visitors intent was? Has already been accomplished. There's no way of knowing what their intent in gathering your pages is/was. You can speculate on you log patterns at best.
Was "NT 5.1 / MSIE 6.0" the entire UA?
Hmmm... I looked more at the UA strings and there is both MSIE 5.5 and 6.0 listed, and both XP and Windows 98. Still don't know what to make of it.