I would love to see the return of Cloak and Dagger in comics, and as they have a history with Spiderman, they could fit well into this idea. The fact that they tend to exist outside the normal perameters of superheroes could work well. Together, they could act as the team's transport and healer, respectively.
I'd suggest Black Cat, who seems to switch between being a villain and a hero every time she appears, so would have no problem pushing the limits of what's acceptable for heroes to do, and would make a good love-interest Superior Spiderman (better than Mary Jane, ugh). She would also fill the espionage/spy-master role usually filled in Avengers by figures like Black Widow, Fury, etc.
I agree the Alpha would be a good choice, as he would be an excellent powerhouse of the group (I'm seeing him as a combination of Thor and Hulk's role), and there is already the foundations of a good teacher/student relationship there.
As for the sixth member... I don't know. Maybe Morbius, who would introduce the more supernatural elements of the Marvel Universe, and would thus act as a foil for the highly scientific Octavius? Or Striker from Avengers Academy (I know that he has nothing to do with Spiderman, but he's all about fame and fortune, and could see this as an oportunity to get in the spotlight if this were a more high-profile group)? Or perhaps even a member of the Slingers (Ricochet, Hornet, Dusk, or Prodigy), who all have a connection with Spiderman?
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