For quality of subtitles for watching an Anime i would go with a Ghibli movie like Sorachan suggested (or anything that has been professionally published, like DVD's in a store) as you can assume that the quality of the Subtitles are very good considering it has been marketed for sale.

For learning Japanese, actual lessons are best. But immersing yourself by watching Anime, Japanese movies is good for providing learning in how to hear and pronounce Japanese