Substitution of the pillaring ligand in the homochiral open-framework [Ni-2(L-asp)(2)(bipy)] by extended bipy-type ligands leads to a family of layer-structured, homochiral metal-organic frameworks. The 1D channel topology can be modified by the nature of the organic linker, with shape, cross-section and the chemical functionality tuneable. In addition, the volume of these channels can be increased by up to 36% compared to the parent [Ni-2(L-asp)(2)(bipy)]. The linker 1,4-dipyridylbenzene (3rbp) gives access to a new layered homochiral framework [Ni-2(L-asp)(2)(3rbp)] with channels of a different shape. In specific cases, non-porous analogues with the linker also present as a guest can be activated to give porous materials after sublimation. Their CO2 uptake shows an increase of up to 30% with respect to the parent [Ni,(L-asp)(2)(bipy)] framework.