A novel nonlinear frequency conversion process was demonstrated to realize the synchronized dual‐wavelength emissions at 1534 and 1572 nm by the mixed optical parametric oscillation (OPO) conversion in gray‐tracking‐resistance KTP (GTR‐KTP) and KTA crystals. Both the two crystals were inserted into the diode‐pumped Nd:YAG/Cr4+:YAG fundamental resonator, with their Y axes perpendicular to each other. This could eliminate the competition of the two OPO processes in fundamental radiation. Furthermore, the ratio between the length of GTR‐KTP and KTA has also been specially designed to satisfy the same OPO thresholds. The synchronized dualwavelength lasing with the power ratio of 1:1 between 1534 and 1572 nm was successfully realized. At an incident LD pump power of 7 W, the maximum total output power of 460 mW was achieved, with the corresponding pulse width and repetition rate measured to be 3.9 ns and 5.5 kHz, respectively. This mixed conversion opens a new door for the multi‐wavelength lasing. (© 2011 by Astro Ltd., Published exclusively by WILEY‐VCH Verlag GmbH & Co. KGaA) (© 2011 by Astro Ltd., Published exclusively by WILEY‐VCH Verlag GmbH & Co. KGaA)