I used the rustolium for all the touchups on my '67 (body shop used chassis black epoxy) and it matched very well. I used it for the firewall and frame too.
I'd say at a minimum you should wire brush and wipe clean with grease remover before painting. I would not paint over anything that you can remove as it will not last very long.
I agree with chief that it may be more expensive with the rattle cans, but it is easier doing one area at a time like you describe.
I used to be indecisive. Now I'm not sure. I feel like I am diagonally parked in a parallel universe. 1968 400 convertible (Scarlet) 1976 T/A - 455 LE (No Burt) 1976 T/A New baby, starting full restoration. 1968 350 - 4 speed 'vert - 400 clone (the Beast!) 1968 350 convertible - Wife's car now- 400 clone (Aleutian Blue) (Blue Angel) 2008 Durango - DD 2008 GXP - New one from NH is AWESOME! 2017 Durango Citadel - Modern is nice! HEMI is amazing! 1998 Silverado Z71 - Father-daughter project 1968 400 coupe - R/A clone (Blue Pearl) (sold) 1967 326 convertible - Sold 1980 T/A SE Bandit - Sold