PokéBase - Pokémon Q&A
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I sent out Palkia after using several Ultra Balls, Pokéballs, a Level Ball, and a Nest Ball, and then I used a Love Ball and it worked. This happened twice. I am confused because Palkia is genderless, and I'm convinced it wasn't just luck.

Last night I achieved what you just attempted in 2013, in Ultra Moon in the "Ultra space wilds" my method was just throwing Premier Poke-balls at it 1x rate you could try poke-balls as they are cheaper to obtain. The reason I went with a Premier ball instead of a regular pokeball was because, Shiny Palkia would look good still in a Premier poke-ball. So I had 4 Love balls in stock, So I said why not throw the love ball at it, as it almost got caught the last time. As you imagined it worked: theory is luck, but also judging how close you are at catching it with another pokeball. You can almost sense you are getting closer. And take a chance, but make sure you have extra balls for what you have planed.

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1x, the exact same as a pokeball
>The Love Ball (ラブラブボール Love Love Ball) should be used on a Pokémon of the same species and opposite gender as the player's Pokémon

This means that Love Ball will only work if the wild Pokemon is of the SAME Species - so that means, you're using a charmander, the other Pokemon must also be a charmander, of the opposite gender for the 8x effect of love ball to take affect. Since obviously you weren't meeting another Palkia in the wild, and also because Palkia is genderless, Love Ball was being a Poke Ball.

So indeed it was luck, like it or not. I once caught a Mewtwo in HeartGold with a Friend Ball after throwing about 50 assorted balls including dusk and ultra balls.. so luck, ftw!

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Love balls work better when your Pokemon is the opposite
gender of the wild Pokemon. You caught Palkia by luck.
Its like capturing a Lugia with a normal pokeball.

No, what I meant was, I sent out Palkia to catch two Pokémon, and I caught both with a Love Ball, after failing with a bunch of other balls.
Ohh sorry