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Would I get better results with a nature that boosts Sp. Attack or Speed?

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Compound Eyes + Thunder is a better strategy than Electro Ball -- but Galvantula usually runs max Speed either way, so it can take full advantage of its good speed tier.

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Damage is roughly proportional to special attack, so a +SpA nature will always raise damage by about 1.1 times.
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Speed and base power work differently with electro ball. They use a table with only 5 possible values, so sometimes you can increase speed and get no change in base power.
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In this example, the user and target have 359 and 199 speed, respectively. A +SpA nature increases damage a little, but a +Spe nature has no effect on damage.

252 SpA Jolteon Electro Ball (60 BP) vs. 0 HP / 0 SpD Perrserker: 133-157 (47.3 - 55.8%) -- 78.5% chance to 2HKO
252+ SpA Jolteon Electro Ball (60 BP) vs. 0 HP / 0 SpD Perrserker: 145-172 (51.6 - 61.2%) -- guaranteed 2HKO
252 SpA Jolteon Electro Ball (60 BP) vs. 0 HP / 0 SpD Perrserker: 133-157 (47.3 - 55.8%) -- 78.5% chance to 2HKO

In this example, the user and target have 359 and 189 speed, respectively. A +SpA nature increases damage a little, but a +Spe nature increases damage a lot.

252 SpA Jolteon Electro Ball (60 BP) vs. 0 HP / 0 SpD Crustle: 111-132 (39.5 - 46.9%) -- guaranteed 3HKO
252+ SpA Jolteon Electro Ball (60 BP) vs. 0 HP / 0 SpD Crustle: 121-144 (43 - 51.2%) -- 5.9% chance to 2HKO
252 SpA Jolteon Electro Ball (80 BP) vs. 0 HP / 0 SpD Crustle: 148-175 (52.6 - 62.2%) -- guaranteed 2HKO

And in both examples, electro ball is weaker than thunderbolt. When you use electro ball, make sure you have a good reason not to use thunderbolt.

252 SpA Jolteon Thunderbolt vs. 0 HP / 0 SpD Perrserker: 198-234 (70.4 - 83.2%) -- guaranteed 2HKO
252 SpA Jolteon Thunderbolt vs. 0 HP / 0 SpD Crustle: 166-196 (59 - 69.7%) -- guaranteed 2HKO

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That dwarfs my answer!  Great answer!
Thanks sumwun! I already had chosen a +Sp. Att. nature but it was to help the other moves.