I am guessing a bit here so sorry this isn't a definitive answer.
I have heard of the old spanish mausers needing to be babied a bit. The ammo sounds like it's at fault here though so your plan to try some hand loads is a good move. I'd bet with a starting load of 2206H or 2208 that you won't get the progessively heavier bolt vs 70yr old surplus that could be degrading, spiky, or generally too hot for the gun. I'd give the bore a good deep clean before you head back out, focussing on the chamber area in case there's a carbon ring building up. Make sure it's dry as a bone in there.
What was the weight of the projectiles in the surplus and what's the twist of the barrel? That or a shot out bore is all that really explains tumbling. If it's borderline then it might not be noticeable on every shot. Might need to go to 130gr or flat base if the gamekings don't work out.
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