HTTWWW has more energy. Just compare the two versions of Rock and Roll. HTWWW blows away the version from TSRTS.
I leave it to Jimmy - he said in the liner notes that HTWWW was Led Zeppelin at its best.
Both albums have great songs that the other one does not, so it would be difficult to choose on that basis.
It was a revelation to me to hear HTWWW when it was released, since I grew up with the original TSRTS and had the entire set memorized. Of course the remastered and expanded TSRTS is magnificent.