We report electrical bistability in electrostatic assembly of CdSe nanoparticles. We obtained thin films of the nanoparticles via layer-by-layer electrostatic assembly technique, which provided a nanoscale control to tune the thickness. Devices based on such thin films exhibit electrical bistability along with memory phenomenon. The bistability is due to charge confinement in the nanoparticles. Conduction mechanism changes from an injection-dominated to a bulk one during switching from a low-to a high-conducting state. Additionally, results from impedance spectroscopy show that the dielectric constant of the material increases during the transition. Both random-access and read-only memory applications are observed in these systems.