Why Am I running unexpectedly hot?

It's hard to get my mind wrapped around your setup from your explanations it would help if you provide a picture of your setup, but with the information you have provided I'll try to help you.

First delidding the 4770K could end up worse than the performance before delidding if the adhesive that secured the IHS in the first place was not dealt with when the new thermal compound was applied, the adhesive itself defines the gap, so are you sure you have good underside contact of the removed IHS and the core die?

The adhesive will hold the contact off of the underside off a little from the CPU die so you need to be sure what's going on under the heat spreader? Do You?

Second water bubbles are bad, you need to get them completely out and it's mostly done by slowly rocking your system back and forth, (With the reservoir sealed of course), to get all the air out of the system, air is an insulator not a conductor , that's why air in your loop is very bad.

It appears you are running your CPU and GPU on the same loop, Is that correct?

It's a first for me hearing of anyone running one water cooled GPU and one air cooled GPU, personally I think that is a bad idea, you should have both either air cooled or water cooled? Especially overclocking!

Do you have plans of changing that or leaving it that way?

Now the biggest problem I see all the time is fellow users attempting a high overclock of an Ivy Bridge or Haswell CPU, the hotter CPUs of the Intel choices, and add the GPUs heat to the loop! That's just flat out bad and not going to help you reach your overclocking goals!

You would never have delidded your CPU if you were not after high overclocks of it , but then you added heat to it from the GPU? Do you understand what I trying to get across to you?

The GPUs added heat idle and load, will seriously limit your CPU overclock! Period no ifs, ands, or buts, to it, and it happens all the time, simply because most are building their systems today on old information that covered CPUs that got no where near as hot as yours does!

So that part is not your fault!

I suggest running 2 independent cooling loops especially if you ever think you'll actually reach the 5ghz CPU overclock goal you have, and water cooling both GPUs not just one.

So what is your response?

For the record I run 2 independent water loops and right now my CPU idle temperature is 16.5c and the load temperature is 41.5c running chilled water cooling at a 5ghz overclock of my (Not Delidded) 3770K.

My GPU, a radiator water cooled GTX Titan idle temperature is 25c and it's load temperature is 34c with a 23c ambient room temperature.

I did not post these results to rub salt in the wound but for you to understand that a properly cooled system has significantly different temperature results.

http://www.tomshardware.com/forum/id-2196038/air-cooling-water-cooling-things.html