By means of quantum-mechanical modeling approach a complex of electrorheological properties of new generation of “smart materials”, i.e., electrorheological suspensions (ERS) on polyimid nanosized particles have been discussed. Optimal structures of polyimides with high value electrorheological response have been prognosticated by the authors on previous stages of work. First in wide range of rheological parameters variation (shear rates. frequencies of periodical sinusoidal low amplitude deformation, temperatures, by different concentrations of disperse phase, etc.) have been taken some important rheological characteristics, namely, flow curves, dynamical rheological dependencies – storage and loss modules, tangent of mechanical losses for ERS on polyimides base. “Giant” electrorheological effect and very week temperature influence up to 80oC for above materials in compare with traditional ERS on microsized particles base has been marked. The results under consideration have wide perspectives for practical using of such type ERS materials.