Flower-like CoMoO4/MnO2 heterostructures have been prepared directly on Ni foam with outstanding pseudocapacitive performance. The heterostructure electrode yields a high capacitance and superior cycling stability performance. Furthermore, the as-fabricated asymmetric supercapacitor device based on CoMoO4/MnO2 positive electrode and activated carbon (AC) negative electrode can operate within a maximum potential of 1.6V delivering both high energy density and power density, which are better than that of the CoMoO4//AC, MnO2//AC, and AC//AC bared density. In addition, the CoMoO4/MnO2//AC asymmetric supercapacitor device demonstrates highly stable cyclic performance with outstanding and robust flexibility. These encouraging results show great potential in developing energy storage devices by building heterostructure nanomaterials.