Adsorption can be used as a pollutant removal method to solve the increasingly serious problem of synthetic dye pollution and metal organic framework (MOF) is considered as a novel adsorbent for its unique structure. However, the high cost and high toxicity during the synthesis procedure of MOFs like MIL-101(Cr) limited their potential on the large-scale production and application. In this paper, waste PET plastic was depolymerized to prepare terephthalic acid (TPA) as an organic linker to synthesize MIL-101(Cr). Besides, Hydrofluoric acid (HF) was not added during the synthesis to avoid poisonous pollution. MIL-101(Cr) was applied to the adsorption of anionic dyes reactive red 2 (RR2) and reactive blue 19 (RB19). The batch experiments exhibited kinetic data best fitted the pseudo-first-order model (PFO) with the adsorption capacity of 662.87 (RR2) and 863.67 mg/g (RB19). The isotherm adsorption data fitted well with the Freundlich isotherm, indicating formation of multilayer coverage over the surface of MIL-101(Cr). The highest regeneration rate of MIL-101(Cr) at the fourth cycle was 91.18 and 91.44 % after RR2 and RB19 adsorption. X-ray photoelectron spectroscopy (XPS) technique and Fourier Transform Infrared (FTIR) spectroscopy both indicated the possible adsorption mechanism of MIL-101(Cr) toward RR2 and RB19 could be attributed to electrostatic interactions, hydrogen bonding, and the π-π stacking. This work proposed a novel method using waste plastics as raw materials to synthesize eco-friendly pollutant adsorbent, which had an enlightening effect on pollutant treatment.