PokéBase - Pokémon Q&A
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I know it can fail.

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Critical Capture

A totally new mechanic of capture is
the Critical Capture. This feature
works like Critical Hits in battle
where there is a slight chance that
this feature occurs. Critical Capture
will be noticed when you throw the
Pokéball. It'll pause in mid-air and
make a metal noise. When it hits the
Pokémon, it will shake once and
capture. This cuts two of the four
random calculations out of the overal
capture mechanic making it more likely
to capture the Pokémon. However, it
can still fail.

The calculation is done by a simple
factor depending upon the amount of
Pokémon species you have captured. It
will run this calculation based upon
the capture value calculated above and
will then have another random number
based upon the Pokémon you have
captured.

Critical Capture =
floor((255,CatchValue) * Multiplier)
The multipliers are as follows;

Table

Pokémon Caught Figure
600+ ------------ 2.5
450 - 599 ------------ 2
300 - 449 ------------ 1.5
150 - 299 ------------ 1
30 - 149 ------------ 0.5
0 - 29 ------------ 0

Or just look right Here where I got all of the information from.

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J98, do you know if by Pokemon Caught, what is meant is Pokemon in Pokedex or actual number of Pokemon caught? For example, would having caught 600 Patrat in Black version make the multiplier become 2.5?
Yes, its the amount of pokemon you've caught, not different pokemon, it can be the same, even something with a crazy easy catch rate.
that kinda sucks 0_o