I would not advise trying to loosen this connection with the eccentric nut as you may be on the rotation side where you’re crushing the pulley into the gantry. I am guessing that, through your adjustments, you backed the eccentric nut out of the black plate on the front a bit pushing your laser out and into square with the bottom cutting surface. The problem there is you may have issues in the future with the nut moving back in and creating slop in the system. I’m guessing if you tightened that 3mm pulley bolt properly, you’d pull it back out of square but all parts would then be secure. There’s no mechanical bits here to adjust tilt.
The only way to fix the tilt securely is shims.