Metal‐organic frameworks (MOFs) are known for their versatility in terms of their crystalline structure, porosity, resistance to temperature, radiation damage, and luminescence among others. Gadolinium (Gd) is one of the elements with the highest reported cross‐section for low energy neutron capture, producing internal conversion electrons and γ rays as a result of the neutron absorption. The development of Gd‐BTC films (BTC=1,3,5‐benzenetricarboxylate) is shown that were deposited on Si and Al substrates by airbrushing, and characterized by profilometry, Raman, EDX and X‐ray diffraction. Radiation damage, thermal decomposition and neutron absorption of these films were studied as well. Gd‐BTC films were attached to CMOS devices (Complementary Metal‐Oxide‐Semiconductor), which are sensible to the internal conversion electrons, in order to build a neutron detector. The devices Gd‐BTC/CMOS could selectively detect neutrons in the presence of γ rays with a thermal neutron detection efficiency of 3.3±0.1 %, a signal to noise ratio of 6 : 1, and were suitable to obtain images.