Gen I has the weird thing where critical hit ratios are based on Speed, so fast things like Jolteon and Dugtrio could score critical hits almost all - if not all - of the time. The ratio did get doubled between Gens 5 and 6, and now there are a few ways to have a 100% critical hit ratio (usually involving Focus Energy) in X and Y.
Also, Frost Breath and Storm Throw have 100% critical hit ratios but I'm assuming you're not counting those.
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