Title: “Headphone Actor” | Artist: Jin feat. LiSA | Anime: Mekakucity Actors
Here’s one that isn’t technically an opening or ending, but an insert song. Mekakucity Actors was a pretty wacky anime at best, but the music it was based on (yes, it was based on music) was excellent, and for the anime Jin had artists such as LiSA lend their vocal strength to the tunes. This was my personal favorite.