Seven new structures were synthesised using a flexible benzimidazolone diacetic acid linker and Mg, Ca, Sr, Ba, Mn, Cu and Zn. The data included consist of structural information (.cif files), bulk phase purity analysed by PXRD (.raw), TGA (.txt), IR (.txt) and NMR. A series of new group 2 coordination networks, MgL = {MgL(H2O)(DMF)0.75}∞, CaL = {CaL(DMF)2}∞, SrL = {SrL(H2O)0.5}∞ and BaL = {BaL(H2O)0.5}∞, were synthesised using a flexible benzimidazolone diacetic acid linker (L) in which the two carboxylic acid binding sites are connected to a planar core via {-CH2-} spacers that can freely rotate in solution. In a ‘curiosity-led’ diversion from group 2 metals, the first row transition metal salts Mn2+, Cu2+ and Zn2+ were also reacted with L to yield crystals of MnL = {MnL(DMF)(H2O)3.33}∞, Cu3L2 = {Cu3L2(DMF)2(CHO2)2}∞ and ZnL = {ZnL(DMF)}∞. Crystal structures were obtained for all seven materials and all materials were also characterised by powder X-ray diffraction (PXRD) and thermogravimetric analysis (TGA). The dataset included consist of structural information from the crystal structures(.cif files). The bulk phase purity was analysed by PXRD (.txt), TGA (.txt), IR (.txt) and NMR. The PXRD files consist of columns for values of 2theta (˚) and intensity (arbitrary units). TGA data consists of columns for time (seconds), unsubtracted weight (milligrams), baseline weight (milligrams), program temperature (˚C) and sample temperature (˚). N.B. The approx. gas flow and R25 diagnostic temperature column are not required. IR data consists of columns of wavenumber (cm-1) and transmission value (%). NMR data files contain the 'fid' file that is needed to open the data in NMR software.