The wide use of alizarin red S (ARS), a typical anthraquinone dye, has led to its continued accumulation in the aquatic environment, which causes mutagenic and carcinogenic effects on organisms. Therefore, this study focused on the removal of ARS dye by adsorption onto a magnetic chitosan core-shell network (MCN). The successful synthesis of the MCN was confirmed by ATR-FTIR, SEM, and EDX analysis. The influence of several parameters on the removal of ARS dye by the MCN revealed that the adsorption process reached equilibrium after 60 min, pH played a major role, and electrostatic interactions dominated for the ARS dye removal under acidic conditions. The adsorption data were described well by the Langmuir isotherm and a pseudo-second order kinetic model. In addition to the preferable adsorption of hydrophobic dissolved organic matter (DOM) fractions onto the MCN, the electrostatic repulsive forces between the previously adsorbed DOM onto MCN and ARS dye resulted in lower ARS dye removal. Furthermore, the MCN could easily be regenerated and reused for up to at least five cycles with more than 70% of its original efficiency. Most importantly, the spent MCN was pyrolytically converted into N-doped magnetic carbon and used as an adsorbent for various dyes, thus establishing a waste-free adsorption process.