Chrysler was famous for building "combination engines" back then. Meaning that everything was designed to work together for BEST results. What that means in that you'll can upgrade the cyl heads to the 1.74" exhaust valves with appropriate stiffness valve springs. Which will put you with a '68-spec set-up (one reason the post '66 383 2bbls were rated at 290 horsepower from the earlier 270 horsepower (using the 256/260 cam rather than the 252/252 of prior times), plus the larger exhaust valves.
A cam with something like the '67 440/375 cam would help, too, teamed with the '68 Road Runner 383 spec torque converter AND related hi-upshift governor for the trans. Plus a good dual exhaust system to complete the replicated "combination" of the '68 Road Runner 383 specs.
I suspect the cyl heads' valve guides will need some attention as a part of the possibly needed valve job. So, with them off, you can physically "cc" the chambers to determine the true compression ratio of the particular motor (which could be a bit less than what the Chrysler rating might be). But they'll probably need to be "surfaced", best done with a mill rather than a "rotating rock" surfacer. The formula to figure that is in many places.
In our Mopar Club, we had a bunch of guys with factory OEM spec cars. When tuned and driven correctly, even with the OEM HP exhaust manifolds, they were extremely hard to beat at the drag strip! One tried to go with "more cam" and the car went slower ET wise, but was faster through the traps. On street tires. So he went back to "stock" HP cam, where he was to start with. A more consistent "pull" rather than "top end rush" which didn't make up for what was lost on the bottom end of things.
Lunati has some "modern version OEM HP cams" which look pretty nice. BUT in a heavier car, with reasonably stock gearing, looking for more torque is better than chasing 6000rpm horsepower, by observation. Which gets to the orientation of "a torque motor that will make power at 5000rpm".
Enjoy!
CBODY67