I'm thinking of trying for something a little unorthodox, want to know if it can be done.
No. Headbutt is a HGSS (Gen 4) Move Tutor Move for Jigglypuff, and Heal Pulse is an egg Move that it can only receive starting in Gen 6. Since Headbutt cannot be passed down to Jigglypuff through breeding, it is impossible.
No. Headbutt can only be learned in gen 4, and Heal Pulse only in gen 6. there's no way you can hatch an egg in two different gens.