We extend the π-orbital space (PiOS) method introduced for planar π-conjugated molecular systems [J. Chem. Theory Comput. 2019, 15, 1679] to also allow constructing efficient π-orbital active spaces for non-planar π-conjugated systems. We demonstrate the performance of this method with multiconfigurational and multireference calculations on prototypical non-planar π-systems: cycloacenes, short carbon nanotubes, various conformations of the 2,2-bipyridine anion, and C20 fullerenes.