I haven't listened to either album in years, but if I was go and dig out one of them now I would listen to the Black Album. I don't really like Megadeth that much now but Countdown To Extinction is decent enough I guess. It has some decent songs such as 'Skin O' My Teeth' and 'Symphony Of Destruction' but then again it has 'Sweating Bullets' which I think is just terrible.
I really enjoyed the Black Album when I first heard it, it was my first metal album actually. I've heard 'Enter Sandman' and 'Nothing Else Matters' more times than I can stand but the album has some really good songs such as 'Sad But True', 'The God That Failed' and 'The Struggle Within'. Although the album isn't the band's best it doesn't deserve all the slack it gets, it still kicks the ass of a lot of metal albums today.
Megadeth - 2
Metallica - 1
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