For me the '60s and '70s produced some of his best more thoughtful work: Time Enough for Love, I Will Fear No Evil, Stranger in a Strange Land, The Moon Is a Harsh Mistress. Though he was beginning to get a bit self indulgent with regard to his social and political views.
His later stuff I have generally found go too far into the self indulgence. Though there are one or two that I liked; Friday was a fun romp.
You've picked my favorites there. I always knew you were a discerning character.