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Existing studies on electro-active polymers (EAP) have largely ignored the unequal-biaxial deformation instability, focusing instead on the equi-biaxial deformation instability of such a material class. The present study develops the first thermo-electrostrictive unequal-biaxial deformation instability model for particle-reinforced EAP composites filled with suitably added filler, which enhances its performance. The model first calibrates the particle-reinforced electromechanical material-oriented data in conjunction with previously released experiments. Later, the model demonstrates several unstable failure modes of the composites, namely thermal absorption, tension loss, electrical breakdown, electromechanical instability, and stretch rupture. Analytical findings of the model solution also manifest the stable and unstable zones of studied polymeric composites undergoing thermo-electromechanical unequal-biaxial deformation in conjunction with all unstable failure modes. Such findings of the proposed model have significant implications for soft robotics, particularly in forecasting the behavior of EAP-based smart composites used in the design of more advanced and efficient soft robotic systems. • An overlooked thermo-electrostrictive unequal-biaxial deformation instability model for EAP composites is developed. • A second law of thermodynamics-based continuum mechanics approach is followed. • Several unstable failure modes of EAP composites are demonstrated. • The stable working areas of EAP composites undergoing thermo-electrostrictive unequal-biaxial deformation are displayed. [ABSTRACT FROM AUTHOR]