@slaw3
After doing a lot of reading on the excellent and very informative discussion on the Steve Hoffman website regarding tube rolling in the LM 508, I tried the EML XLS 300B tubes, which are excellent and definitely a step up from the stock tube. I replaced the 6SN7 tubes with some 1940s vintage Sylvanias from Brent Jesse, which were also terrific.
I have tried a two or three 6SL7 tubes, settling for now on a Mullard ECC35--it is a bit on the pricey side, but sounds great. I think the finesse of this tube is a nice complement to the robust dynamics of the EML 300Bs.
So far, I have stuck with the stock 805 tubes. I may roll in some others at some point, though what I would really like to try would be some Elrog 300Bs. These are REALLY pricey, so it may be a while before I can experiment with these.
I am not sure I can say which change would result in the biggest difference, but I would certainly suggest trying some different 300Bs. Before you do anything, spend some time reading the Steve Hoffman thread. There are several 508 owners there who have done a lot more tube rolling than I have in their amps. You might benefit from their experiences, as I did.
The 508 is a good amp even with the stock tubes, but you can definitely take it higher by finding a combination of tubes that suits your particular tastes.
Happy listening!