Complete series
I SPY (all 82 episodes on DVD as well as I SPY RETURNS made 25 years later)
THE PRISONER
THE RICHARD PRYOR SHOW
THE BEN STILLER SHOW
THE VEIL
Incomplete series
THE TWILIGHT ZONE (original series, Definitive Collection -- first 2 years)
THE TWILIGHT ZONE (1980s) -- First season
THE OUTER LIMITS (1960s -- I bought the first season but not the second yet).
THE OUTER LIMITS (1994-2001 -- only 14 episodes out of 152)
NAKED CITY --- 28 episodes on 7 discs from the 2nd, 3rd, and 4th seasons. The second year was the first as an hour-long show. No half-hours on DVD yet.

DANGER MAN (a.k.a. SECRET AGENT) -- I haven't purchased the 39 half-hour episodes from the first season yet. So far I only have about a dozen or so of the 45 hour-long ones from the second and third.
THE WILD WILD WEST --- I have the first 10 discs, which includes the entire first season (black & white) and first 3 episodes of the second season (color).
KOJAK (first season)
IN LIVING COLOR (first 2 years, buying the third season next week)
COLUMBO (1970s) (both pilot movies including "Prescription: Murder" made in 1967 and the first 2 years 1971-73)
WISEGUY --- 49 out of 75 episodes. The rest are not yet on DVD including "Wiseguy Returns" TV movie sequel.
ANGEL --- First season only so far. I haven't gotten around to buying Buffy the Vampire Slayer at all, but I've seen every episode of both series in first-run.
CHAPPELLE'S SHOW --- First season
SLEDGE HAMMER! --- First season, and I'm buying the second / last soon.
THE RED SKELTON SHOW / THE RED SKELTON HOUR -- I have several of these which are public domain, including 1 color episode from 1970 guest starring John Wayne.
GUNSMOKE --- Most of the black & white hour-long episodes from the 1960s, which I disc-recorded off-air 4 to a disc from The Westerns Channel.
SATURDAY NIGHT LIVE --- Several complete 90 minute episodes from the 1970s, 80s, and 90s I disc(ed) off-air from NBC All Night.