LLC is basically supplementary voltage. Cpus are almost never under a constant load, it varies multiple times per second. Each change will show up on a graph as ups and downs, this is vdroop, the difference between the peaks and valleys. If the valley droops too far, there's not enough voltage for the load the cpu is trying to work and you get instability. LLC is a supplement to the droop, pre-emptive, so the cpu will actually get what it's needs to use.
But it's very touchy, too much LLC is just as bad as too little, can't just stick it on level 5 or extreme or 100%. There's 2 major voltages associated with a cpu. Vcore and VID. LLC affects both. VID is what the cpu demands from the motherboard VRM's, vcore is what it actually uses, so vcore and VID should be within about 0.05v of each other. Adding LLC too high means overall the cpu uses more than what's demanded and you get instability. Setting VID high to compensate means you cook the VRM's in attempting to supply that voltage.
So most OC will happen around level2-3 or med-high or 50-66%. Extreme/100% is basically only for those doing extreme OC, LN² off the charts kinda stuff.
It's a balancing act, combined with the ripple from the psu, you just want to compensate, not replace.