TOP round is SHOT; headstamp should tell you what size. They were for revolvers for bird-shooting, worked okay at close range but REALLY spread, often gave a donut-shaped pattern. You used to be able to get them in quite a few sizes: .38 S&W Long (which I think this might be), .44-40, .38-40, .45 Long Colt are the ones I have seen. This one is pushing 100 years old, so don't bang it off!
Pics 2 and 3 are a British-made bolt for the Number 4 Rifle, Mark 1 or 1* doesn't matter; there was no difference in the Bolts.
Pic 4 is an array of ammo in chargers. Top left is a Springfield 1903 charger with 5 rounds of original .30US M-1906, it looks like: white-jacketed bullet is made of cupronickel; all the later types (M-1, M-2) used copper-colored slugs, so this is early, likely War One stuff. Maker's name and date on the base. There is a charger there (far left) which is a British Mark II type, so early War One. Also chargers of Rounds and Brass both, likely War One, possibly as late as War Two. Check the rounds very carefully and give us the markings on the case-HEADS as well as a side elevation; could be xome nice Specials in there (looks so by the different Crimps: Ball Mk VII all was crimped halfway down the Neck)
Pic 5 is 2 rounds of .41 Swiss for the Swiss Vetterli rifles: rimfire, 10.35mm, paperpatch bullet. Goes $8 a round and up. You also have a 20mm projectile (HE) for the Hispano or Oerlikon cannon. Lots and lots of these released on the open market, unfilled and LOOKING very live, up into the 1960s. Some also had a Trace element in the base. Likely inert but don't toss it in the fire, just in case. Fuse assembly just unscrews for filling; you sometimes find them filled with a kind of sand and painted green. This one still is shiny and so likely factory-unfinished, surplus by the ton and now a hard-to-find little item.
BOLT is for a .22, but I don't know anything about them apart from Cooeys. Think this could be Savage.
Hope this helps.