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Is there a known way to go about this?
I have a zillion expansion fish that I have a 0% chance to desynth, and at 74 skill right now nothing but rare ARR fish seem to offer any boosts. Sky fishing does work, but at 0.01 per catch. Pirarucu offer some (0.10?) but the catch rate is low.
Got a fishing retainer? That's the only thing I can think of - send them out for a fish you would rather not catch. Collect a bunch of them and then start desynthing away.
Alternatively, spend 3k gil each on the item over in the Silver Bazaar, that is used for the Zodiac quest. Desynth that and level up a ways on it. Not too sure that you can recoup your cost on it anymore though.
If i remember correctly, I used the giant clams from the lucis quest to level my desynth up to 100
I did Silver Sovereign's (sp?) around that level until close to/around 90, then moved onto the crowned pies (mass bought the items required for them via GC seals). About 105 on-wards 3.0 fish started becoming very efficient IIRC.
I used a Tinkerer's Calm and Bacon Broth combo (careful desynth +4). Both items are expansion quest rewards, so they should be pretty cheap on the market. As soon as I noticed a 7%-10% success rate on the expansion fish, I just bought up a bunch of cheap fish from the market board, and shamelessly burned them. If I remember correctly, you should be able to get to 120-130 on blueclaw shrimp alone.