You can do that just fine with a couple cautions.
First off, the tolerance on the original caps was -10% - +90% (or 50% in a few cases). So the original caps could have been anywhere between 36 uf and 76 uf and been in spec!
Second, you do have to respect the limits of the tube rectifiers. The C11 A and B caps can't go much larger without jeopardizing the 5U4s - so you can use 100 uf total, but no more. In fact, if the original caps were even 25% above spec, they would have had 100 uf of capacitance. 100 uf is fine there - but higher than that is not wise.
On the C6A and C6 B caps - you can use pretty much as large a cap as you want - but the law of diminishing returns applies. Those caps decouple the low level and PI stages from the main B+ along with R10 and R21, so I'd make R10 & R21 2 or 3 watts to be sure they run cool. If it was me I'd use a dual section 100/100 cap. I might even parallel a 4-5 uf film caps with each section. That's a healthy increase, it's easy to install, and will make a nice sonic improvement. 500 uf is likely overkill, 200 uf or so is god.
Don't forget to replace C7 - the bias cap; replace the selenium rectifier too! There you could use 100 uf as well. And the cathode bypass on the 1st 6CG7 (C3) should be replaced too. Use 50 uf at 35 volts or higher for there.
Let me know if you have any questions. I'll try to help if I can.