TV:
Cross Game - Sports, but really slice-of-life and romance. Simple perfection from the genius, Adachi.
AnoHana - check with me again in three weeks, but as of now one of the best and most moving dramas you'll see.
House of Five Leaves - Seinen (I guess). A period drama about a kidnapping ring and a hapless but kind samurai. Slow-paced but gorgeous, and an exquisite character study.
FMA: Brotherhood - As fine a shounen adaptation start to finish as I've seen.
True Tears - Arguably the best romance anime of the last half-decade.
Natsume Yuujinchou - Two seasons (third on the way) of youkai and emotionally moving stories about loneliness.
Movies:
5 Cm Per Second - The most visually beautiful anime ever IMO, and the first part is one of the most simple and beautiful love stories.
Colorful - A magical realism tale about a soul given a second chance at life, via the body of a 14 year-old suicide victim. Gritty, honest and ultimately uplifting.
Summer Wars - Spectacularly imaginative story about family dynamics and social networking gone haywire.