When your temps are up, touch bare metal on the PSU to ground yourself, then check to see if the blocks are hot to the touch. Of course, you don't want to let the CPU or GPU get too hot, so keep an eye on the temps while you are checking the blocks.
If the blocks are cool when your CPU and GPU temps are over 60C, then you have a large thermal barrier between the processors and the blocks. The heat is not getting to the blocks, hence something must be wrong with the mount.
If they are very warm, then the heat is getting to the blocks, but for some reason, the coolant isn't transferring the heat to your radiator. Likely causes are poor coolant flow and air or gunk insulating the block from the coolant.
Did you rotate the blocks to get the air out? Is there air elsewhere in the system? Is the tubing kinked? Is the pump on? Does it work? Did something get into the system and plug it up? I'm not sure if the head loss for running water backward through a jet impingement block would be enough to drive your GPU temps up as much as you're seeing, but the lack of jets would drastically affect the CPU temps.
If the radiator is hot, then you need to figure out why it's not transfering heat to the air. This seems unlikely to be your problem, though.