In this paper, two kinds of metal organic frameworks (MOFs), MIL-53(Al) and MIL-53(Al)-NH2, were synthesized. Then these MOFs were used to remove methylene blue and malachite green dyes from aqueous solution. Characterizations of MOFs were carried out by X-ray powder diffraction (XRD), scanning electron microscope (SEM), Fourier transform infrared (FT-IR) spectrometry, and zeta potential. Experimental results showed that MIL-53(Al)-NH2 can rapidly bind to the two kinds of cationic dyes from aqueous solution with high adsorption capacity. However, the adsorption capacity of MIL-53(Al) for cationic dyes is extremely low. The adsorptive selectivity of MIL-53(Al)-NH2 to the cationic dyes resulted from the hydrogen bonding interaction between amimo groups of the dyes molecule and the MIL-53(Al)-NH2, while the extremely low adsorption capacity of MIL-53(Al) for the dyes may be main caused by the "breathing" behavior of MIL-53(Al). The factors including adsorption time, temperature, and the pH of solution that affected adsorption of the two dyes on MIL-53(Al)-NH2, were studied. Pseudo first-order kinetic, pseudo second-order kinetic, and Weber Morris models were used to fit the adsorption data, and the pseudo second-order kinetic model showed a better fit for the adsorption of methylene blue and malachite green than that of the pseudo first-order kinetic model. Furthermore, the internal diffusion model which represented by Weber-Morris model was involved in the step of speed control, but it was not the only speed control step, while out-diffusion also played an important role in the adsorption process. The adsorption isotherm and thermodynamics of methylene blue and malachite green on MIL-53(Al)-NH2 were also studied. The adsorption of methylene blue and malachite green dyes on MIL-53(Al)-NH2 can be fitted to both Langmuir and Freundlich isotherm, but the former was better than the latter. The adsorption thermodynamic experiments demonstrated that adsorption reaction was spontaneous and endothermic. Finally, according to the experimental phenomenon, the possible mechanism of adsorption was proposed. Besides, the used adsorbent can be reused for adsorptive removal through simply washing.