the harlock series is in the same boat as the 999 series. the first 26 episodes of the 42 episode series have been subbed.
most of the new series have all been licensed so subs are readily available.
the best old school harlock is the movie "arcadia of my youth" and is licensed.
the rest of the 999 movies have been subbed, most are available commercially. (i think the first two are unlicensed)
the first two (of three) yamato series are subbed, as well as the movies. i don't think the third series is available subbed.