Cancer has recently begun to occur very commonly in humans, and the number of new cancer cases and deaths is also increasing year by year. To reduce these numbers, the development of new materials, which have the potential to be used for both diagnostic and therapeutic purposes, is very significant for sensitively detecting and effectively destroying cancer cells. Therefore, this work purposes the development of gadolinium‐based metal‐organic frameworks (Gd‐MOFs) via solvothermal method under various conditions such as the use of different ligands types, the presence or absence of PVP and variable ligand/metal ratios, and the preparation of silica‐coated and 10B modified Gd‐MOF nanocomposites to fabricate as the potential candidate for simultaneous uses in MRI and the combined neutron capture therapy (GdNCT and BNCT) applications. The XRD patterns of Gd‐MOFs showed the formation of [Gd2(BDC)3(DMF)2(H2O)] structures with 1,4 H2BDC ligand and [Gd(BTC)] structures with 1,3,5 H3BTC ligand. In the presence of PVP by using the least amount of ligands, experimental ligand/Gd ratios were calculated as 1.52 and 1.06 for [Gd2(BDC)3(DMF)2(H2O)] and [Gd(BTC)], respectively, which are very close to theoretical ratio. After the silica coating and 10B modification, the surface appearance of the prepared nanocomposite changed in general, and Gd/10B ratio into nanocomposite was calculated as 3.0, indicating that it could be a useful candidate for the simultaneous GdBNCT and MRI applications.