Full Metal Alchemist, Brotherhood, not to be confused with Full metal alchemist
A 40 plus episode story that is well plotted with a few twists and a satisfying ending.
A ton of characters that are pretty well developed, a few very powerful bad guys with one big bad, a long history and a really long final battle between good and evil for the souls of everyone and it all starts with a journey by two boys to try and regain what they lost whilst using alchemy and its biggest taboo.
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Starts off lulling you into thinking its really girly stuff being about magical girls but ends up being a well crafted, very dark story, some have labelled it Lovecraftian and I can see where they are coming from.
Like Evangelion, it is seen as a deconstruction of its genre.
Gurren Lagaan and Kill la kill are batshit crazy takes on the Mecha and magical girls genres, Gurren Lagaan probably being better but Kill la kill is funnier, both do complete flips a good way in, turning the stories in directions you never saw coming.
Baccano, Darker than Black, From the New World, Ergo Proxy, SteinsGate, are all good too, not going to list everything I like
Movies, well there are so many.
Sword of the stranger is simple but superbly well done.
Paterma inverted is a nice watch for a family anime movie.
A silent Voice an anti-bullying movie and Your Name is a body swap story with a great twist, I did read that JJ Abrams bought the movie rights to this.