Marked For Death is very useful, but must be used with caution when you have followers. I use it on dragons a lot. Or enemies shooting at you from a distance. Just shout and watch them die.
It took me a long time before I understood the point of Become Ethereal, but when I did - yes, me like!
Fire breath is good against trolls and in dungeons with oil on the floor

Unrelenting Force always works.
Kyne's Peace is great when you don't feel like fighting wildlife all the time. There's a cave crawling with spiders and only spiders in Eastmarch, this shout made that cave easy-peasy. And you really only need one word of it, if you're just using it to get past the animals.
And Slow Time is beginning to be a new favorite of mine, allowing me to get a few extra strikes on Deathlords before they hit me. Even with only one word.