Energy-dispersive X-ray spectroscopy (EDS) combined with SEM showed that the elemental composition of the sheaf superstructures (major product) and the rods (minor product) are similar (Figure ). The different components: carbon (from the ligand), nickel cations and chloride anions are homogeneously distributed. Micro-Raman spectroscopy revealed that the vinyl-pyridine moieties in both types of morphologies coordinate to the metal centers (Figure ). The intensities of the pyridine ring bands of the ligand at ν = 992 cm -1 and 1001 cm -1 are blue shifted to ν = 1008 cm -1 and 1025 cm -1 , respectively, as expected for the formation of pyridine-Ni 2+ complexes. The composition and the coordination chemistry were confirmed by X-ray photoelectron spectroscopy (XPS) of the bulk (Figures S4c). The nickel cations retained their oxidation state (+2). Two distinctive peaks at 855 eV (2p3/2) and 872.5 eV (2p1/2), and the satellite bands (for 2p3/2 = 859-869 eV and 2p1/2 = 876-886 eV) can be attributed to the 2p orbitals of Ni. The signal for N is present at 400 eV (1s), and the bands for the counterions Cl (-1) were observed at ~199 eV (2p3/2). For comparison, the signal of the nitrogen atoms of the free ligand appears at 399 eV (1s), and for Ni of NiCl2 at 856 eV (2p3/2) and 873.5 eV (2p1/2). These shifts are indicative of the coordination of the vinyl-pyridine moieties to the nickel cations. These observations imply that the sheaf superstructures (major product) and the rods (minor product) are structurally equivalent. ). The 3D framework is formed by coordination of four pyridine moieties from four different CSB ligands and two Cl anions with the bivalent metal center. The six ligands and the metal cation form octahedral geometry. The pyridine moieties of the achiral ligand are arranged in a propeller-type, chiral arrangement, possibly to minimize the steric hindrance between adjacent ligands. The four Ni-N distances of 2.090 Å, 2.094 Å, 2.096 Å, 2.108 Å, and those of Ni-Cl (2.493 Å) are well within the ranges normally found for NiX2(pyr)4 (X = halide). The structure has two different nanochannels with an opposite chirality (P and M that run in parallel to the c-axis. The pore size is 7.5 Å × 6.4 Å and the framework contains 41% solvent accessible voids of the total volume (calculated by Mercury CSD 2020.1.1).