Most of my favorite champs are the outlandish, inhuman ones, and that generally translates to my skin choices as well. Void Fizz made me particularly happy, as did everything about Vel'koz when he released. Hazmat Heimer is also looking swanky, despite mystery gifts landing me with every skin he has up to this point already :P ( I don't know why, but I've always loved the look of gas masks. Apocalyptic Brand and Hextech Singed were also very nice in that regard!) And, like most people, I love me some fancy top-hats, so I have a soft spot in my heart for Magnificent Twisted Fate and Superb Villain Veigar, though Bad Santa is also pure gold :P
As far as sets of skins go, I've made it my goal to collect all of the Robot skins, and I've yet to be disappointed in anything that's come from them. All of the Battlecast and Mecha Skins are just beautiful, Full Metal Rammus's Powerball and ult are so much more intimidating than base, all that jazz... If I were to complain about any of them, it might be that Battlecast Xerath doesn't mesh well with the rest of the skins in the set, but I've seen that brought up more than a few times around here, so I doubt it's new information to you people on the Skins team!
And now for skin ideas, because I'm sure you don't have enough of your own already and this seems like a worthwhile place to dump them! I'll try and avoid concepts I've already seen from other people, particularly if Reds have commented on them in the past.
Jurassic Skarner: Because we already know (or at least assume) that the currently-lacking Void champs will be getting their entries into this set some day down the line, why not show some love to others who fit the mold? Skarner strikes me as a prime candidate for something almost like a Trilobite, still partially fossilized with some parts of his body more indentation than physical remains. Doesn't strike me as something that would specifically need unique particles in any way, but like his other two skins, it's far more interesting than a recolor!
Janitor Fizz: Perhaps a tie-in to the Jurassic skins? Giving Fizz a mop (and the requisite Scruffy-esque mustache, of course) is a small enough change, but then make Chomper a megalodon skeleton and everything is awesome and right with the world!
Mad Chef Shaco: I know the guy's slated for a visual and mechanical rework so I can't speak to any specific effects, but if he retains his dual-wielding ways, it just seems obvious to give him a carving knife and a cleaver, matching bloody chef's hat and apron, and possibly a terrible French accent.
Prickly Rammus: Apparently Blitz matched him correctly, as Rammus' offspring is a living, walking cactus in the shape of an armordillo! Cacti and bramble bushes sprout up around him when he ults, and he leaves a small trail of cactus blossoms in his wake as he powerballs around!
Haunted Pantheon: Something I've been surprised hasn't come up much in the past, but the Faceless Spartan just seems like the perfect candidate for a skin slating him as a possessed suit of medieval armor, decked out with a flamboyant tower shield and halberd. Depending on how much you played up the ghostly visual effects, I imagine there would be plenty of play-space available for fun animations and particles.
Cataclysmic Xerath: A walking (floating?) apocalypse. Literally a swirling vortex of death and destruction given partially-human form. Q is lightning bolts, W is erupting geysers of lava or steam, E is hurled debris (bonus points if they're mooing cows a small percentage of the time), and R calls down meteors from on high to bombard the unworthy!