This work reports an environmentally benign and readily scalable process for production of akaganéite (β-FeOOH) nanocomposites by using abundant gallic acid or grape seed tannins and urea. Influences from those phytochemicals on the properties of β-FeOOH nanocomposites were investigated by X-ray powder diffraction, Fourier transform infrared spectroscopy, Thermogravimetric analysis, Scanning electron microscopy, Transmission electron microscopy, UV–Vis spectroscopy and Photoluminescence. The addition of 0.1% (w/v) grape seed tannins or gallic acid (640 mg L−1) solution yielded single-crystalline β-FeOOH nanocomposites with reduced dimensions, increased porosities and BET surface area, and no oxidized impurities such as hematite (Fe2O3) were formed. The added grape seed tannins (S0.8) or gallic acid together with less urea (0.8 M) produced β-FeOOH nanocomposites with higher activities as peroxidase mimics compared to those prepared with only urea (C0.8). Moreover, S0.8 was more efficient in methylene blue (MB) discoloration compared to C0.8 at all three pH values of 4, 7 and 11, and the S0.8-mediated MB degradation pathways at pH 4 and 7 were different from those at pH 11 due to the generation of different predominant oxidants. The overall MB discoloration efficacies by S0.8 at pH 4, 7 and 11 were combinative effects of both physical adsorption and chemical reactions. These β-FeOOH nanocomposites possess great potential as peroxidase mimics for facile monitoring of excess hydrogen peroxide and applications in environmental remediation. Display omitted •Grape seed tannins applicable in hydrothermal synthesis of β-FeOOH nanocomposites.•Grape seed tannins produced smaller β-FeOOH nanocomposites with improved porosity.•β-FeOOH showed improved peroxidase-mimic activities for methylene blue discoloration.•Methylene blue degradation underwent different pathways with a change in pH.