My best guess would be that those 61 are intended to be “solo” monsters. Legendaries, dragons, and other monsters the designers expected to most often be used as bosses. Does that jibe with the 61 you observed to have the higher hit chance?
Oh, no, no, no! That's not what's going on at all (clever guess from my scanty info though!)
You probably already know this, but I'll briefly explain for anyone following. There are only 4 values that go into the equation that produces CR: HP, DPR, AC, and AB. That's it. There most definitely are many other factors that effect CR, but the way they do it is by altering those 4 values into the effective values that actually end up being plugged into the equation.
The DMG describes what, for purposes of the not terribly accurate DMG version of the monster building rules, those other values are that alter the basic 4 and what alterations they make. The official CR calculator spreadsheet's data entry page seems to show that at least some of those alterations are similar to the real monster math, but not all of them are.
Exactly how all of those alterations to the basic 4 values are done is unknown. In order to figure that out out, we need to first discover the correct equation, and then test--as far as is possible--each alteration independently.
Those 61 basic monsters are all of the monsters that I can be sure have no features that would affect their HP, DPR, AC, or AB. They just have the raw stats and nothing that might modify them. No saving throw bonuses. No damage resistances or immunities. No features that cause you to make a saving throw, or impose a condition. Etc. They are your "boring bags of hit points". Many of them are beasts. None of them have a CR above 7. Honestly, if there were as many monsters like that as people think there are this would be a lot easier to do! (It's actually likely that there are other monsters whose additional features have no effect on CR, but from the input form and info we do have, and lacking the full instructions of how to use that form, I can't be sure.)
So what's the importance of the basic monsters? Limiting initial trials of proposed equations to them is the only way to make sure the equation works right. The correct equation should work on 100% of basic monsters. Then I can move on to trying to discover how all the other variables actually adjust the 4 basic values, in order to fully reverse engineer the math.
However, I'm stuck at 95% of those monsters, and can't find any way to do better.
The 2 monsters that won't work with anything I can even think of are the twig blight and the needle blight. They both always come out weaker than the CR the MM gives them, regardless of what variant of what equation I use. Since they were in the original Starter Set that predated the MM by like half a year it's possible that they hadn't refined all the math (and, AFAIK, they never change the listed CR of a monster after publication), or even that they just decided to cheat, because they preferred that the CRs of the three blights ended up as the published 1/8, 1/4, and 1/2, rather than the 0, 1/8, and 1/2 they probably actually are by the official math. If it's the latter, it's quite possible they did that before they decided to stop doing that and be strict about using the results the equation gives them--which I think they have been doing since the MM.
The other anomaly depends on which equation I use. I've developed several which end up with only 3 failures, but can't get it down to just those blights. The one I posted also fails on the grimlock--which is the most common one to take that honor. I have no explanation whatsoever for it. It just doesn't come up with enough XP to push it into the listed CR 1/4. Now, there are some equations that will get it there, but they are at least a little more complicated, and instead fail on different monsters. The one I'm most comfortable failing on is the myconid sprout, because there is an easy mistake that could have been made when entering its data that could cause it. But again, it just seems like the equation(s) that give us the grimlock as an inexplicable failure are more likely to be accurate.
So that's what those 61 basic monsters are and why they are absolutely critical to everything--they are the ones that all have to work.