Probably my favourite of his poems is "She dwelt among the Untrodden Ways", which is about an ideal woman, only recognised by the poet. It deals with unrequited love.
I also quite like "Strange fits of passion have I known", which is about the poet journeying to his lover's cottage, each stanza dealing with his varying thoughts upon the way. Anyone who has ever travelled to a loved one's home with empathise with the rising excitement and trepedation of the poem.