It was clearly an Adjucha lizard during Ichigo's training with the Vaizards. This Adjucha lizard fought without the conscious direction of Ichigo or Shirosaki, but were only fighting captain level shinigami whom didn't even release their swords [except for Kensei].
Then, he appears again right before Ichigo dies from his chest wound with Orihime's screaming and Ulquiorra in his second stage Resurrection, and proceeds to hand Ulqy's arse to him with undeniable superiority. The heaviest reiatsu displayed in Bleach so far (according to Ishida anyway) was defeated by this newly seen hollow form that came from Ichigo's power, and again it wasn't even directed by Ichigo or Shirosaki's mind, thus it's undeniably Vasto Lorde hollow transformation.
I think Ulquiorra is Vasto Lorde afterall. He's just weaker then 1-3 because he didn't make the high speed regeneration for greater powers trade!
I believe Shirosaki could've defeated Ulquiorra with his Adjuchas Lizard body too though.