Developing new adsorbents with hierarchical pore and unsaturated adsorption sites are highly demanded to achieve rapid adsorption rate and good adsorption selectivity in purifying organic wastewater. We here reported a new Quasi-MIL-125(Ti) synthesized at 340 °C under air atmosphere and considered as a high-efficiency adsorbent for capturing cationic dyes. The morphology of the material is characterized by XRD, SEM, TEM, etc. and the adsorption performance of Quasi-MIL-125(Ti) was systematically studied. Remarkably, it takes only 1 min to rapidly remove 20 mg L-1 MB or NR with 1 g L-1 Quasi-MIL-125(Ti), which is far superior to the previously reported materials. Adsorption isotherm shows that dyes adsorption on Quasi-MIL-125(Ti) follow a Langmuir adsorption isotherm model. The experimental maximum adsorption capacities were 109.3 mg g-1 for MB and 151.1 mg g-1 for NR, respectively. The hierarchical pores facilitate the diffusion and co-adsorption of different dye molecules. Adsorption mechanism reveals that the strong electrostatic attraction originated from the unsaturated Ti sites in Quasi-MIL-125(Ti) contributes to the ultra-fast adsorption behavior during cationic dyes chemisorption process. This study not only provides a promising prospect for the synthetic strategy of super-adsorbents, but also provides reference and theoretical guidance for practical dye wastewater treatment.