I'm sure that there'll be No Way Home Marvel Legends figures of Doc Ock, Goblin, etc. at some point but it is worth noting that those Toy Biz Spider-Man movie figures were basically Marvel Legends caliber already, especially the ones released for Spider-Man 2.
There really isn't a whole lot of room for improvement even after almost 20 years but it would still be awesome to see updated sculpts. Maybe all-new versions of Sandman, Venom and Black Suit Spider-Man too since those Spider-Man 3 Marvel Legends figures that Hasbro did back in 2007 weren't really up to par. That was when they were still in their transitional period after they picked up the Marvel license before the sculpts improved.