They are the worst because they are single pack and extremely slow drying. It’s very very old technology, nitrocellulose is essentially the first spray paint. It will absolutely react with all chemical release agents, as well as any tooling system containing a solvent like styrene or MEK. It is also quite toxic, as well as potentially explosive. Personally I would throw it away, it’s horrible stuff. That said, you COULD use it to make a mould if you were to use PVA as your release agent and spray it on very thick so there can’t be any reaction between the paint surface and the tooling gelcoat. Or use it to practice your spray painting technique, you could respray a crappy old car or something. Just don’t spray anything that you care about the finish on!
As for 2k paints, they come in a variety of chemical bases from polyester to urethane to polyurethane to epoxy. Just be careful using epoxy, single pack epoxy paints are somewhat more common than two pack epoxy paints, and these are also not suitable for mould making. 2k paints are a spray paint, they are used in exactly the same was as any other spray paint including your nitrocellulose. They are simply resins that require a hardener to cure, but because they have a hardener they do actually cure hard unlike unlike 1k paints which simply dry by solvent evaporation and will always remain ‘soft’.