In this work, we introduce a simple and effective method for the controlled release of dye from dye saturation flocs by a well-designed pH responsive chitosan-based flocculant. The dye flocculation capacities could be precisely controlled from 0.5 to 2 g g⁻¹ by simply adjusting the pH of the desorption solution. A series of flocs with different dye flocculation capacities was prepared and used as nitrogen-rich precursors to prepare nitrogen-doped carbon materials through one-step carbonization. The results demonstrate that the specific surface areas, pore structures and supercapacitance performance of the resulting N-doped carbon materials could be readily controlled by varying the dye flocculation capacity. By using a dye sludge floc with an appropriate dye flocculation capacity (1.5 g g⁻¹) as a precursor, the resulting N-doped material exhibited a high specific capacity and good cycling performance for a supercapacitor electrode. The unique pH-responsive properties of the chitosan-based flocculant facilitated easy tuning of the surface cationic degree and deprotonation behavior by varying pH. This work presents a new concept for balancing between environmental capacity and energy capacity using a smart pH-responsive carrier system based on modified chitosan, which is highly promising for the recycling of industrial wastewater to produce energy materials.