Simultaneously polarimetric radar (SPR) realizes the rapid measurement of a target’s polarimetric scattering matrix by transmitting orthogonal radar waveforms of good ambiguity function (AF) properties and receiving their echoes via two orthogonal polarimetric channels at the same time, e.g., horizontal (H) and vertical (V) channels (antennas) sharing the same phase center. The orthogonality of the transmitted waveforms can be realized using low-correlated phase-coded sequences in the H and V channels. However, the Doppler tolerances of the waveforms composed by such coded sequences are usually quite low, and it is hard to meet the requirement of accurate measurement regarding moving targets. In this paper, a joint design approach for unimodular orthogonal complementary sequences along with the optimal receiving filter is proposed based on the majorization–minimization (MM) method via alternate iteration for obtaining simultaneously polarimetric waveforms (SPWs) of good orthogonality and of the desired AF. During design, the objective function used for minimizing the sum of the complementary integration sidelobe level (CISL) and the complementary integration isolation level (CIIL) is constructed under the mismatch constraint of signal-to-noise ratio (SNR) loss. Different SPW examples are given to show the superior performance of our design in comparison with other designs. Finally, practical experiments implemented with different SPWs are conducted to show our advantages more realistically.