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When Harribel is killed, during her flashback Apacci comments saying that Harribel was a Vasto Lorde.

So I am wondering who of Aizen's Arrancar were Vasto Lorde

Memor-X
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It was implied that top 4 of the Espada were all Vasto Lorde level as they were far superior combatwise than a Soul Society Captain. However, out of the four, only Tier Harribel was confirmed as a Vasto Lorde.

Sparsha Bhattarai
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    There's an official side story thingie that shows how Ulquiorra becomes a Vasto Lorde. – zibadawa timmy Oct 30 '17 at 04:37
  • I don't think that Stark and Barragan were just Adjuchas. And we still don't know if Grimmjow was able to become a Vasto Lorde after eating his companions. – Alix Eisenhardt Oct 30 '17 at 10:32
  • Barragan looks like a Vasto Lorde to me. When Aizen went to subdue the so called "Lord of Hueco Mundo", it was shown that Barragan was as humano-like as he can be, considering that his power is that of "time", which is different than Grimmjow. Grimmjow was shown as a panther. – 絢瀬絵里 Oct 30 '17 at 15:41