Coordination polymers of [Zn(INA)2] (1) (INA = isonicotinate), [Cu2(mal)2(H2O)2(bipy)] (2) (mal = malonate, bipy = 4,4‐bipyridine), and [Zn2(OAC)4(bipy)2] (3) (OAC = acetate) were prepared using mechanochemical grinding and heating methods. The materials were characterized with elemental analysis, FT‐IR spectroscopy, TGA, SEM, EI‐MS, BET, and PXRD. Comparison of PXRD patterns of the materials with patterns simulated from single‐crystal X‐ray diffraction data allowed identification of the products. Compared to conventional synthetic techniques such as solvothermal/hydrothermal solvent‐based methods, solvent‐free method was found to be simple, highly efficient, and environmentally friendly especially for the preparation of these coordination polymers on a large scale. Solvent‐vapor interaction properties of 1, 2, and 3 were investigated by exposure of the compounds to water and methanol at room temperature.