The Cover Feature shows the bis(tridentate Schiff base Pt(II)) complex containing dimethyl sulfoxide (Pt2L2DMSO) as a combination of yellow disks, gray disks, orange cones, and a black curved line. Pt2L2DMSO is unfolding due to the steric repulsion of the bulky ligand. The blue hexagons connected to the branched black lines stand for poly(4‐vinylpyridine) (P4VP). The green curved figure in the background indicates hybridization. The top image shows the hybridization of Pt2L2DMSO and P4VP, which causes a ligand exchange reaction for Pt2L2DMSO, forming a folding network structure in the yellow membrane. The yellow membrane exhibits red photoluminescence under ultraviolet irradiation (green wavy arrow). The reddish thunder expresses phosphorescence. The bottom image in the cover shows hybridization of Pt2L2DMSO and 4‐vinylpyridine (4VP), which causes a ligand exchange reaction for Pt2L2DMSO, forming the folding columnar packing structure in the brown block crystal. The black wavy arrow indicates non‐radiative deactivation. The metallofoldamer crystal does not exhibit solid photoluminescence under ultraviolet irradiation, while the metallofoldamer membrane is luminescent, thanks to the hybridization with P4VP. The background color changes gradually from orange to gray at the bottom to orange at the top, showing the improvement of photoluminescence from bottom to top. More information can be found in the Research Article by H. Achira and co‐workers.