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So far, Ho-oh is paralyzed, and only has a slither of HP left.. Nothing works but I really need to catch him.
Ho-Oh is level 70
This is on Pokemon SoulSilver

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master ball
Sorry forgot to say apart from master ball

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Ultra Balls and Dusk Balls

These are your best bets right now. Unless 40 turns have passed.In which you will probably use a Timer Ball
Assuming it has 1HP left (False Swipe) with an Ultra Ball :

You have a 2.833% chance of capturing it per ball. Thus, you have at least a 50% chance of catching it within 25 balls and at least a 95% chance of catching it within 105 balls.

If you are , however, catching it in the Night
Dusk Balls will do better than Ultra Balls

>You have a 5.525% chance of capturing it per ball. Thus, you have at least a 50% chance of catching it within 13 balls and at least a 95% chance of catching it within 53 balls.

Or you can go for a Level Ball.
Since Ho-Oh is level 70 using a Pokemon quater or below 70 will increase Capture Rate by a bit.

>You have a 1.234% chance of capturing it per ball. Thus, you have at least a 50% chance of catching it within 56 balls and at least a 95% chance of catching it within 242 balls.

Or you can just use a Master Ball

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I thought level balls work well if the Pokemon your fighting has a lower level than you. Or is that the nest ball?
Level ball works if your capture target has a higher level I believe.
And Nest ball is lower level