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The old way work well
Spiritbond lv45 to 50 crafting gear
You can do it almost everywhere (during the main quest roulette... Fighting any dark tribe during daily trib quest... Killing water spirit in urth gift...)
It spirit bond in less than 10 minute without potion
Cost nothing
Yield ton of T3 materia (i mean... Like if T3 control are not needed)
And you get pretty oftenly a T4 materia
Last try i did yesterday i got 2 T4 control with à lv46 set
What i did was as follows
1) Get a set of the ilvl100 Crafting gear from Moghome npc including main hand tool.
2) Attach 3 pieces of garbage materia to each piece.
3) Equip the +1 Spirit Bond neck and Wrist from Grand company and two Meteor Survivor rings.
4) FC Spiritbond buff + Better crowned pie and spirit bond potion.
This will bond the gear in 150 quick synths. I grabbed 3 stacks of Rainbow cotton balls off the MB and synth those up followed by turning those into thread.
It's fairly cheap to do and you can make some of the costs of mats back from the thread / cloth you have.