The REAL answer is actually to use all of the information together.
For example, the load range of the tire is based upon its PSI.
So, if the tire says its supports 3000 lb at 40 psi, or 3000 lb at 80 psi...you need to know that.
Its on the sidewalls.
Next, you take 35% of your GVWR, say 5,400 lb as an example (GVWR is on that placard).
35% of 5,400 lb = 1,890 lb.
So, MINIMALLY, you need at least enough psi to support 1,890 lb.
If the sidewall says its MAX is 3000 at 40 psi, you divide 1890 by 3000 and get 1890/3000 = 0.63
So, you need 63% of the max load, and, therefore ~ 63% of the MAX PSI.
If the max psi = 40, then ~ 26 psi would support the 1,890 lb.
If the max psi was 80, then ~ 51 psi would support 1,890 lb
Round up, we ARE talking about finding the MINIMUM PSI, and your GAUGE is probably only accurate to a percent or 3, etc....
(The tire that NEEDED more PSI to SUPPORT ITS MAX WEIGHT, will run at a higher PSI, because it NEEDS MORE)
The above is a great way to ball park the ranges...in real life, tires are not perfectly linear in load range/psi percents, but, are typically within a pound or so...plenty close enough.
Again, the 35% of GVWR is a MINIMUM for psi settings, many people run closer to 40% for example.
So...try the above to see what's about right...at a minimum, you'll be in the ball park, and from there, you can see how you like the ride/handling.
Too bouncy/harsh at the minimum setting...well, its probably just a bad tire match for you.
Too wishy washy for you at the minimum, add 5 psi and try again, rinse/repeat.
The chalk test can be OK, but, its a lot better for bias ply tires than for radials...much harder to tell the difference in the chalk wear with the radials.
Just like torque wrenches, etc...the tire works best at the sweet spot in its range.
Some tires work better at the lower ends of their load ranges, other at the higher ends...but MOST seem to work best between 60 - 80% of their max load, with 75% being a common target.
THAT means that when SELECTING a tire, you should consider its load range, and where ~ 35-40% of YOUR GVWR would fall relative to it.
If POSSIBLE, choose a tire with ~ 75% of its load range being about 35 - 40% of your GVWR....for the best match.
Sometimes, people choose a load range/tire that is simply wrong for their truck...its MAX load might be fine, but they run the tires at too low a PSI to SUPPORT that load....
...or they get a tire that's actually too heavy duty, such that it would be running with the sidewalls bulged out at a PSI you'd need to support the rig's weight, etc....and the handling feels like driving on greased squirrels, the rear comes out on turns, etc.
IE: If the tire is a bad match for your truck/use...there's not much you can do except try to return it...or hope it wears out quickly/try to not have an accident/not have your kidneys pounded into jelly, etc.
Food for Thought.