You can walk anytime, obviously. When I was a student in London, we used to head out at midnight to walk around the city. As well as the streets being clear, there was the added advantage of a bacon sandwich in Smithfield and a free newspaper from Fleet Street (OK, it was a long time ago, I admit).
More relevantly, I have done some excellent walks in the Chilterns well into the evening. In June and July it is perfectly feasible to catch a train after work to Chesham or Amersham and walk for three hours before it is dark. I have done that with a group of friends a number of times (walking around at night on my own doesn't seem like a good idea).
It terms of the best days, weekdays are obviously good because the train service is at its best. Travelling out of London mid-morning allows you to take advantage of off-peak rail fares. Annoyingly though, on the way back, you can be be the only person on a train at 5 p.m. travelling towards London but have to pay a peak fare - because that is the way the fares work.
Sunday can be a pleasant day to walk particularly if you don't have too much else to do. But, beware the fact that trains are slower, less frequent, and you are more likely to be stranded somewhere because of engineering works.
That leaves Saturday, which is probably the best day for most people... and the reason the the estimable Saturday Walkers Club, walks on, er, Saturday. They know what they are doing! They have a tradition of starting their walks fairly early in the morning, though. That is necessary if you want to do a long walk, but not to everyone's taste.
Whatever time you choose. Enjoy your walk!
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