Here are the skills I'd personally love to see in some shape or form in LoL. These are excerpted from the HotS wiki, so don't worry about numbers.
Gilnean Cocktail (Greymane)
Hurl a flask that deals 55 (+4% per level) damage to the first enemy hit and explodes for 220 (+4% per level) damage to enemies in a cone behind them.
This is an unusual skillshot in that, to get the best damage, you don't want to directly hit your intended target but hit them with the explosive cone. The primary target will only take minor damage, but everyone else behind it will take considerably more. Great for poking an enemy who's hiding behind minions.
Lightning Surge (Alarak)
Deal 62 (+4% per level) damage to an enemy and an additional 100% damage to enemies between Alarak and the target. Restore 70 (+4% per level) health for each Hero hit.
Again, you don't want to directly cast this on your intended target. Instead, you want to catch them in between your cast target and you. This makes positioning really important.
Butcher's Brand (The Butcher)
Deal 37 (+4% per level) damage to an enemy and Brand them for 4 seconds. The Butcher's Basic Attacks against the Branded target heal him for 75% of the damage done.
Basic Attacks against Branded Heroes heal for double and extend the duration of the Brand by 0.5 seconds.
This is a unique means of providing sustain. You mark the enemy (you need to be in melee range) and then for a short time, your attacks on a marked enemy heal you significantly. Obviously, there's good counterplay too: kite your enemy until the mark expires, or peel the attacker away from a marked ally.
Apocalypse (Diablo)
Create a demonic rune under each enemy Hero on the battleground. After 1.75 seconds the rune explodes dealing 137 damage and Stunning for 1.75 seconds.
This one's an ultimate ability, and boy is it potent. While it's easy to dodge the rune if he just does it out of the blue, it's during team fights that it becomes truly dangerous, as dodging it becomes much more difficult if you're preoccupied or already CC'd.
I'll add more later.