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Unfortunately, Entei has no set location in Pokemon Crystal - he always moves around. The only time you really 'see' him is in the Burned Tower in Ecruteak City (4th badge). Once you enter the tower, go left, up, right, and down until you see your rival. Battle him. Once you've defeated him, you will fall to the bottom floor. There will be Raikou, Entei, and Suicune. You won't be able to battle any of them, but they'll jump around you and make their leave. After that, it's up to you to find Raikou and Entei.

Usually you'll see them at times you don't expect it on your adventure, but once you see them, you'll have their location in your Pokedex at all times. If you've seen Entei, for example, them go to your Pokedex and see where he is. Go to the area and walk around in tall grass. Use a repel or super repel to keep Pokemon at low levels away - Entei is the only Pokemon you care about. After a while, check where he is again and repeat.

Once you do see him, though, either use a Master Ball or put him to sleep. Entei and Raikou always flee at first chance, and then you have to do it all over again.

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