All done now, and quite a bit has been sampled for scientific purposes.
So, my findings:
Smoking the entire roast before hand at 225 degrees, until the IT hit 150 degrees, provided me with a slightly smoked flavor. The smoke taste was hinted at and not real pronounced. My wife loved the flavor. This was based upon the top rack of jerky that didn't get any smoked salt or pepper added prior to dehydration.
Adding the smoked salt to the top of the still moist slices, prior to dehydration, gave a bit more of a smoke flavor and a nice salty kick. I used low sodium soy sauce and Worcestershire in the recipe and didn't add any salt to the marinade, other than the small amount of cure #1.
Adding the fresh cracked black pepper to the still moist slices, prior to dehydration, will be done from this point forward. Great flavor and not over powering like I've had before when I added it directly to the marinade. Also, quite a bit of the pepper can be easily brushed off once the jerky cooled down, my wife really liked that aspect since she can't do a lot of spicy.
Since I didn't mop, baste, coat, slather, or even season the exterior of the roast prior to smoking it, the outside edges of the dehydrated slices were quite a bit drier than the center portion of the slices.
I'm not certain if I got a really tender eye of round (is that possible), or if the precook made the difference, but this jerky is VERY tender, much more so than what I usually get. I did slice across the grain, but I always do. The outer edges were tough and extremely dry, but the middles are very bite friendly.
The cure didn't help to retain much, if any, of the meat's natural color. When I tore a piece open, it looked like gray cooked meat, the flavor is there, but without the normal cured color.
Will I do it again? Yep! I love experimenting with all things smoker related.
For the next one, I'm contemplating a low salt wet cure in Pop's brine, and then smoking the whole thing, before slicing to marinade.... I travel all next week, so 5 days in the juice is doable!