Simultaneous fully polarimetric radar uses orthogonal polarization channels to transmit a pair of signals, both of which must have good auto- and cross-correlation characteristics. In this paper, the design of sequences with good correlation properties and Doppler tolerance is investigated. New cyclic algorithms, namely, Cyclic Algorithm-Gradient I (CAGI) and Cyclic Algorithm-Gradient II (CAGII) are proposed to solve the optimization problem. Meanwhile, the sequences designed in this paper have ultra-low auto- and cross-correlation side-lobes in a specified lag interval. Numerical experiments are conducted to demonstrate and validate the superiority of the proposed cyclic algorithms, especially for the measurement of moving targets.