Wow...
I think I'll just have a bit of fun with this one. I don't think everyone will like my choices, but I'm going to put them all out there anyway.
Ultimate Spider-Man (Best as an hour long TV series on Network Primetime)
Peter Parker: Liam Aiken (Lemony Snicket, Road to Perdition)
Spider-Man (stunts): Duane Carnahan (kid stuntman + actor, voice dubbed)
Mary Jane Watson: Kay Panabaker (Summerland, Phil of the Future )
Aunt May: Diane Keaton (Family Stone, Something's Gotta Give)
Uncle Ben: John Voight (National Treasure, Glory Road)
Harry Osborn: Tyler Hoelchin (Road to Perdition, 7th Heaven)
Norman Osborn: Hugo Weaving (Matrix, LOTR series)
Green Goblin (Hellboy/Thing-style Suit): Brock Lesnar
J. Jonah Jameson: JK Simmons (who else?)
Gwen Stacy: Hayden Patnierre (Heroes, Remember the Titans)
Doctor Otto Octavius: Ralph Fiennes (Red Dragon, Harry Potter series)
Nicky Fury: Samuel L. Jackson (Is there a discussion here? Really?)
Kraven the Hunter: Duane "Dog" Chapman (Dog the Bounty Hunter)
Ben Urich: Steven Hyde (That 70's Show)
Captain Stacy: Aaron Eckhart (Paycheck, Thank You For Smoking)
Electro: Micheal Rosenbaum (Smallville, JLU)
The Kingpin: James Gandolfini (Sopranos)
Justin Hammer: Ian McKellen (X-Men Series, LOTR Series)
Eddie Brock: David Gallagher (7th Heaven)
I think that'll just about cover the first season. It's made so that high profile actors guest star as villains, for maybe 3-6 episodes out of a 22 episode series. Thus, keeping the show cheap and attracting awesome actors to a high-profile low-commitment project. There may be better choices for some roles, but you get the general Idea.
Ultimate X-Men I would actually prefer this as a cartoon, due to the action and rather straightforward personal plots, nothing deeper than what's seen on JLU or Avatar. While I would do my first voice casting, I think it'd be better to cast live action, perhaps just for cameos sake (not that X-Men cameo too often in other books).
Charles Xavier: James Marsters (Buffy, Smallville... resembles Patrick Stewart. Looks good bald. Owns)
James Howlette: Steven Straight (Undiscovered, Sky High... hair is shorter now... and he owns the dark brooding charisma Wolvie needs).
Scott Summers: Jonathan Bennett (Veronica Mars, Mean Girls... he just works)
Jean Grey: Lindsay Lohan (as much as we hate her, she is a proven actress)
Hank McCoy: I will always claim complete cluelessness here.
Peter Rasputin: Daniel Curdmore (still young, still huge)
Ororo Munroe: Zoe Saldana (Heavn, Guess Who, POTC... name it)
Bobby Drake: Taylor Lautner (Cheaper by the Dozen 2, Adventures of Sharkboy...)
Kitty Pride: Somehow clueless...
Magneto: Viggo Mortensen (LOTR. He would own. I'd follow him anywhere).
Juggernaut: Big Show (WWE)
Toad: Rupert Grint (Harry Potter, Lessons in Driving)
QS and SW: See Ultimates Below.
I still wouldn't know what to do with that series. It should be too expensive for serialized TV, but too extensive for just a movie to do... and the movie's already been done.
The Ultimates Works best as a one shot UBER blockbuster trilogy. Just throw all the money you have at it... say 300 Million USD and watch it soar. Uber Wide Release in all countries, DVD with director's cuts and deleted scenes and specials and colelctors editions and more toys and liscenced clothing than you can shake a stick at. Get double your money back, do it again two summers from now.
Captain America: Brad friggin Pitt (Because everyone loves him an Achilles Owned)
Iron Man: John friggin Travolta (Because he can do just about anything)
Thor: Ralf Moeller (Gladiator, Pathfinder)
Wasp: Lucy friggin Liu (Cuz she's hot... and smart)
Giant Man: Jim Carrey... because GM is a big jerk.
Hulk: Eric friggin Bana (Cuz he knocked it out of the park last time)
Hawkeye: Vin friggin Disel (Because he feeds his kids off of badassness)
Black Widow: Charlize get it-get it Therone (because she's good)
Scarlet Witch: Kate takesallcomers Beckinsdale (because she's hot)
Quicksilver-- Chad Micheal nottooyoung Murray (because QS is a jerk)
Kleiser -- Giovanni Ribisi (Flight of the Phoenix, 10th and Wolf)
And Freddie Prinze Junior as himself
Oh, of course Nick Fury: Samual L. "I'm tired of these M*f*ing snakes on this M*f*ing Plane!" Jackson. Now that's a movie.
Ultimate Fantastic Four Best as a Sci Fi Channel series. Let them do all the trippy things Sci Fi is known for... alternate dimensions... time travel... ancient civilizations... that's UFF to a tee. Same celebrity guest star villains and cameos like before. Use the movie cast as the Zombie FF.
Reed Richards: Jensen Ackles (Smallville, Supernatural)
Susan Storm: Kristen Bell (Veronica Mars, Pulse)(GREAT call!)
Johnny Storm: Hunter Gomez (National Treasure)
Ben Grimm: Somehow clueless. I don't know a whole lot of young big guys...
Victor Van Damme: Wilmer Valderama (That 70s Show, Fast Food Nation)
Dr. Storm: Brent Spiner (Star Trek TNG, Enterprise, Material Girls... THE man for Sci Fi, writing as well.)
Dr. "Mole Man" Molekevitz: Danny Devito
Namor: Randy Orton (WWE) (GREAT call!)
Crystal: Hillary Duff
And that should just about do it for me. Yeah... got no time for much more. Call it as you will.