This work reports on zeolitic imidazolate framework (ZIF)-coupled microscale resonators for highly sensitive and selective gas detection. The combination of microscale resonators and nanoscale materials simultaneously permits the benefit of larger capture area for adsorption from the resonator and enhanced surface adsorption capacity from the nanoscale ZIF structure. Dielectrophoresis (DEP) was demonstrated as a novel method for directly assembling concentrated ZIF nanoparticles on targeted regions of silicon resonant sensors. As part of the dielectrophoretic assembly process, the first ever measurements of the Clausius-Mossotti factor for ZIFs were conducted to determine optimal conditions for DEP assembly. The first ever real-time adsorption measurements of ZIFs were also performed to investigate the possibility of inherent gas selectivity. The ZIF-coupled resonators demonstrated sensitivity improvement up to 150 times over a bare silicon resonator with identical dimensions, and real-time adsorption measurements of ZIFs revealed different adsorption time constants for IPA and CO2.