<p>The contaminations of water resources by toxic heavy metals have extensively emerged from the anthropogenically industrial development due to their persistent and bio-accumulative effect, which gives rise to potentially irreversible toxic effects for aquatic ecosystems and human health. There maintain urgent demands for novel adsorbents capable of efficiently elimination wide ranges of heavy metals in wastewater.&#xa0;The synthesis of high adsorption capacity, low cost, and recyclable adsorbents has become a significant challenge. Herein, the calcined Co-Zn-Al layered double oxides (Co-Zn-Al LDO) and Co-Zn-Al layered double oxides/chitosan-derived carbon quantum dots (Co-Zn-Al LDO-C) were triumphantly prepared using in-situ hydrothermal and calcination methods, and uptake performance toward Cr(VI) was also conducted under various water-chemistry conditions. The recyclable Co-Zn-Al LDO-C hybrids showed unexceptionably physicochemical stability and remarkable adsorption capacity of 2.96 × 10^–3&#xa0;mol/g, which obviously surpassed the reported materials in previous literatures. The kinetic process of Co-Zn-Al LDO-C with ultrafast adsorption rate (within 60&#xa0;min) was in great accordance with pseudo-second-order kinetic model. Based on above discussion results, the especial reductive reaction, cation exchange, surface complexation were primary mechanisms for elimination performance of Cr(VI). The particular XPS spectroscopic analysis illustrated that nitrogen-containing and transition metal element-containing functional groups played significant role in elimination of Cr(VI) onto Co-Zn-Al LDO-C hybrids. The experimental result underscored that the promise of Co-Zn-Al LDO-C hybrids to function as versatile adsorbents, had extensively promising prospect in the remediation of heavy metals contaminants from wastewater.</p>