Reaction of methanolic copper(II) acetate solution with oxazolidine 21 (HL7) led to the formation of the one‐dimensional coordination polymer 1D‐∞1[CuL27] 23. On the contrary, reaction of copper(II) acetate in methanol with pyrrolidine 24 (HL8) yielded the two‐dimensional coordination polymer 2D‐∞2[CuL28] 26. A common feature of 23 and 26 are the C2h‐symmetric coordinatively unsaturated building blocks 22 and 25. In 1D‐∞1[CuL27] 23, the cyano groups are linked to copper in a side‐on fashion and the monomers 22 are oriented parallel to one another, whereas in 2D‐∞2[CuL28] 26 the cyano groups are bound to copper in the end‐on mode and the monomers 25 are oriented at an angle of 117° to one another. In both 1D‐23 and 2D‐26, copper has a distorted octahedral coordination sphere. On the other hand, reaction of methanolic copper(II) acetate solution with enantiomerically pure (5S)‐pyrrolidine 27 (HL9(S)) led to the formation of the diastereomeric helical strands (M)‐/(P)‐1D‐∞1[CuL29] 29. (M)‐ and (P)‐29 are present in pairs in the infinite unit cell. In helical 1D‐29, copper is tetragonal‐pyramidally coordinated and the C2‐symmetric monomers 28 (CuL29) are linked through only one cyano group. Moreover, it has been shown that the reaction of chiral racemic pyrrolidine 30 (HL10(R,S)) with copper(II) acetate via the intermediate Ci‐symmetric building blocks 31 (CuL10(R)L10(S)) furnishes one‐dimensional 1D‐∞1[CuL10(R)L10(S)] 32. Single‐crystal X‐ray diffraction analyses of the supramolecular species 23, 26, 29, and 32 unequivocally establish the structures of these coordination polymers.