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Pyrethroids are common contaminants in water bodies. In this study, an efficient mussel shell-based adsorbent was prepared, the effects of factors (calcination temperature, calcination time, and sieved particle size) on the pyrethroid adsorption capacity from calcined shell powder were investigated via Box–Behnken design, and the prediction results of the model were verified. By characterizing (scanning electron microscopy, X-ray diffraction, Fourier infrared spectroscopy, and Brunauer–Emmett–Teller measurements) the adsorbent before and after the optimized preparation process, the results showed that calcined shell powder had a loose and porous structure, and the main component of the shell powder under optimized condition was calcium oxide. The adsorption mechanism was also investigated, and the analysis of adsorption data showed that the Langmuir, pseudo second-order, and intra-particle diffusion models were more suitable for describing the adsorption process. The adsorbent had good adsorption potential for pyrethroids, the adsorption capacity of the two pesticides was 1.05 and 1.79 mg/g, and the removal efficiency was over 40 and 70% at the maximum initial concentration, respectively. [ABSTRACT FROM AUTHOR]