A new gadolinium(III)-pyridine-2,5-dicarboxylic acid (GdIII-2,5-H2pdc)-based three-dimensional coordination polymer, namely, poly[dimethylazanium [bis(μ-pyridine-2,5-dicarboxylato)gadolinium(III)]], {[(CH3)2NH2][Gd(C7H3NO4)2]}n, CP-1, has been synthesized via a typical solvothermal method. The as-synthesized material was characterized in the solid state using single-crystal X-ray diffraction, powder X-ray diffraction, thermogravimetric analysis and FT-IR spectroscopy. During the synthesis of CP-1, the in situ dimethylformamide (DMF) promotes the formation of a dimeric unit and these act as secondary building blocks in the assembly of a three-dimensional anionic {[Gd(pdc)2]-}∞ framework. The framework has channels along the c axis which are filled by dimethylazanium cations. Interestingly, the framework shows a helical-type assembly running down the a axis. A Hirshfeld surface analysis of CP-1 suggests that extra stability is provided by hydrogen-bonding interactions. The magnetic properties of CP-1 showed weak antiferromagnetic couplings between adjacent Gd3+ ions.