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To truly beat the game you will need to complete the Pokédex. The regional Pokédex is the same as the Pokédex from the Pokémon Red and Blue games. Once you have 60 unique Pokémon registered in your regional Pokédex and beaten the Elite Four, Professor Oak will upgrade your regional Pokédex to the National Pokédex, which includes all the Pokémon from Pokémon Gold and Silver and Pokémon Ruby and Sapphire, making it a total of 386 Pokémon.

Pokédex Certificates

To obtain the regional Pokédex Certificate you need to catch 150 Kanto Pokémon, excluding Mew.

To obtain the regional National Pokédex Certificate you need to catch 380 of the 386 Pokémon, excluding Mew, Ho-Oh, Lugia, Jirachi, Deoxys, and Celebi.

Catching Pokémon

Most Pokémon from the Kanto region are accessible in the wild as you progress through the game. However, there are specific Pokémon exclusive to each version of the game and you will need to trade Pokémon from the complementary version to complete the regional Pokédex.

Pokémon FireRed exclusives
Pokémon LeafGreen exclusives

Legendary Pokémon

These Pokémon will only appear once, so if you defeat them you won't see them again. Save the game before battling them.

Pokémon Location
ArticunoArticuno Seafoam Islands
ZapdosArticuno Power Plant
MoltresMoltres Mt. Ember
MewtwoMewtwo Cerulean Cave

Legendary Beasts

You can only obtain one Legendary Beast, depending on which starter Pokémon you chose. You will need to trade with other players for the two you didn't obtain.

Pokémon Starter Pokémon
RaikouRaikou Squirtle
EnteiEntei Bulbasaur
SuicuneSuicune Charmander

Available from NPCs

Although not available in the wild, certain Pokémon are available by interacting with characters in the game.

You can only obtain these Pokémon by trading with specific NPCs:

Obtain Location
Farfetch'dFarfetch'd Vermilion City
LickitungLickitung Route 18
Mr. MimeMr. Mime Route 2
JynxJynx Cerulean City

During the game, you will collect an Old Amber in Pewter City and either a Dome Fossil or a Helix Fossil in Mt. Moon. Taking these to the Pokémon Lab on Cinnabar Island will allow you to regenerate Aerodactyl, Kabuto and Omanyte respectively. As you can only collect Kabuto or Omanyte, you will need to trade with another player for the one you didn't obtain.

These Pokémon will be given to you as you progress through the game.

Obtain Location
HitmonleeHitmonlee or
HitmonchanHitmonchan
The Fighting Dojo
EeveeEevee Celadon Mansion

Breeding

You only receive either Hitmonlee or Hitmonchan from the Fighting Dojo, and Hitmontop is not available at all. To collect all 3, you will need to breed the one you have with a Ditto to produce a Tyrogue. Once it reaches level 20, it can evolve into one of the 3 evolutions based on his stats:

Evolution Stats
HitmonleeHitmonlee Attack higher than Defense
HitmonchanHitmonchan Defense higher than Attack
HitmontopHitmontop Attack equal to Defense

There are 5 possible evolutions of Eevee, so you will need to breed the Eevee you are given with Ditto four times.

Evolution Requirements
FlareonFlareon Fire Stone
JolteonJolteon Thunderstone
VaporeonVaporeon Water Stone
EspeonEspeon Level up during the day with high friendship
UmbreonUmbreon Level up during the night with high friendship

Trading

To obtain the National Pokédex Certificate you will need a Pokémon Emerald or Pokémon XD: Gale of Darkness game to obtain the Johto starters and trade them to your FireRed/LeafGreen game.