Furfural residue (FR) is an inevitable by-product of industrial furfural production. If FR is not managed properly, it will result in environmental problems. In this study, FR was used as a novel precursor for activated carbon (AC) production by H3PO4 activation under different conditions. Under optimum conditions, the prepared FRAC had high BET surface area (1,316.7 m2/g) and micro-mesoporous structures. The prepared FRAC was then used for the adsorption of Cr(VI). The effect of solution pH, contact time, initial Cr(VI) concentration, and temperature was systematically studied. Characterization of the adsorption process indicated that the experimental data were well-fitted by the Langmuir isotherm model and pseudo-second-order kinetics model. The maximum adsorption capacity of 454.6 mg/g was achieved at pH 2.0, which was highly comparable to the other ACs reported in the literatures. The preparation of FRAC using H3PO4 activation can make use of FR's characteristic acidity, which could make it preferable in practical industrial production.