Tough choices..... I didn't include partially-released series sets in this list.
My #1 would be tied with the CBS Fugitive series if S2-3 hadn't been affected by the music edits.
1) Combat!
2) Time Tunnel
3) Dick Van Dyke Show
4) Six Million Dollar Man
5) Twilight Zone (Definitive version)
The Fugitive gets a big honorable mention but my set includes a mixed set other than the CBS set so it's not on this top 5 list
I didn't include miniseries in the 1st list but with those included, it would look like this:
1) Combat!
2) Time Tunnel
3) Rich Man, Poor Man miniseries (both "books")
4) Shogun miniseries
5) Six Million Dollar Man, edging out the Twilight Zone (Definitive version) set by a nose. The deciding factor in my #5 pick in this list was that everyone's waited years for the 6M$M set and the TZ sets have been available for years prior to the T/L 6M$M set. The other reason is a "shout out" to Matt for his contributions to the 6M$M set, as well as Joe Burns and Jim Sherrard.