I'd personally say the most evil acts in the series are:
1) Ramsay's treatment of Donella Hornwood.
2) The deaths of Aegon and Rhaenys.
3) Tywin's destruction of the Reynes. (due to how over-the-top his methods were)
4) Randyll Tarly threatening to kill Samwell.
5) Victarion murdering his wife for being raped.
What do you think?
Raid on Saltpans and Sack of Tumbleton with multiple victims. Torture of Theon, Rape of Jeyne and , although semi-canonical, what Rorge did to Biter