In this work, for the first time, magnetic binary metal oxides nanocomposites which integrated Zr and Ti into one entity on an atomic scale on polydopamine coated magnetic graphene (magG/PD/(Zr-Ti)O-4) was designed and synthesized, and applied to the enrichment of phosphopeptides. The newly prepared magG/PD/(Zr-Ti)O-4 composites gathered the advantages of large surface area, superparamagnetism, biocompatibility and the enhanced affinity properties to phosphopeptides. MagG/PD/ZrO2, magG/PD/TiO2, as well as the simple physical mixture of them were introduced to compare with magG/PD/(Zr-Ti)O-4 composites. High sensitivity (1 pg/L or 4.0 x 10(-11) M) and selectivity (weight ratio of -casein and BSA reached up to 1:8000) toward phosphopeptides were also presented for magG/PD/(Zr-Ti)O-4 composites. Additionally, mouse brain tissue was chose as the real samples to further investigate the phosphopeptides enrichment ability of this new material.