In the present work, a facile method for the preparation of nanocomposite adsorbents composed of carbon and iron compounds was demonstrated. The adsorbents were produced by pyrolyzing an iron-coordinated 1,8-diaminonaphthalene at various temperatures under an N2 stream (FeDN X, where X represents the pyrolysis temperatures 600, 700, and 800 °C). Prepared FeDNs were employed as adsorbents for the removal of Cr (VI). The Cr (VI)-adsorption behavior of FeDNs were well-fitted to a Langmuir isotherm model. Among the samples prepared, FeDN 700 showed the best performance for the removal of Cr (VI). In particular, the maximum adsorption capacity of FeDN 700 was evaluated to be 34.81 mg/g. A variety of characterizations were carried out to elucidate the relationship between physical properties of adsorbents and their adsorption behaviors.