A novel dual-mode analytical method by employing nanozyme was developed for the detection of organophosphorus pesticides (OPP) for the first time. The detection principle is that the pesticide could be hydrolyzed to para-nitrophenol (p-NP) in the presence of nanoceria as nanozyme. p-NP exhibits the bright yellow color, and its color intensity has a positive correlation with the pesticide concentration. Meanwhile, the characteristic absorption peak at 400 nm of p-NP increases gradually with the raised concentration of pesticide. Therefore, a dual-mode method including smartphone-based colorimetric and spectroscopic strategies was rationally developed. Herein, methyl-paraoxon was selected as the representative compound. Under the optimum conditions, the detection limits of both two strategies were calculated to be 0.42 mu mol L-1. Finally, the present method was successfully applied in three edible medicinal plants (Semen nelumbinis, Semen Armeniacae Amarum, Rhizoma Dioscoreae). The present work offers a reliable and convenient approach for routine detection of pesticide based on two different detection mechanisms.