Ternary transition metal sulfide (TTMS) contains numerous metal active sites, rendering promising adsorbents. However, a challenging problem in their further applicability is how to expand the available active surfaces which hindered by aggregation. Here, a novel strategy of engineering hybridization of CuFeS2 with boron carbide nitride (BCN) nanosheets was proposed vis an in-situ facile controlled hydrothermal process. An improved specific surface area of approximate 6.24 times enlargement was achieved for TTMS of CuFeS2 under the uniformly dispersion effect of BCN nanosheets. Meanwhile, the fabrication of nanocomposites CuFeS2-BCN significantly enhanced the adsorption affinities including hydrogen bonding, π-π interactions, metal-complexation and electrostatic interactions, thereby resulting in an amazing elimination capacity of 90.72% which respectively 25% and 368% growth toward pristine CuFeS2 and BCN for antibiotic contaminant of chlortetracycline (CTC). Systematic adsorption studies of adsorption kinetics, isotherms, and thermodynamics revealed that the adsorption process of CuFeS2-BCN-0.1 to CTC was spontaneous and endothermic, and followed the pseudo-second-order kinetics and Langmuir isotherm models. The maximum Langmuir adsorption capacity was super high and up to 1166.31 mg/g, which was superior to the majority of the reported adsorbents. In addition, it is also worth emphasizing that the nanocomposites of CuFeS2-BCN-0.1 possessed satisfactory selectivity, stability and adaptability to many tetracycline antibiotics in multicomponent solution under diverse pH environments. All of these findings presented that the proposed advanced adsorbent of CuFeS2-BCN-0.1 displayed great promising application potential in the treatment of antibiotic contamination wastewater.