Coordination polymers (CPs) are gained numerous investigations due to their structure talents, such as ultrahigh high specific area, abundant pores or channels, and diverse and adjustable composition in energy storage area. However, their application on supercapacitor devices is restricted by low conductivity and lack of stability. In this work, a Co- and benzenetricarboxyl-based CPs (Co-BTC) is selected as precursor, and then used as template to fabricate a layer-double-hydroxide-covered core-shell structure (noted as Co-BTC@LDH) using a cation/anion co-exchanging process. This fine tune nanomaterial is achieved by, which demonstrates a remarkable specific capacitance of 1226 F g−1 at a current density of 1 A g−1, and outstanding ratio performance of maintaining 86.79% initial capacitance even as the current density elevates tenfold to 10 A g−1. Moreover, the as-fabricated asymmetric supercapacitor based on Co-BTC@LDH and active carbon (AC), displays an energy density of 58.70 Wh kg−1 at the power density of 0.36 kW kg−1 and an impressive cycle stability of retaining 98.2 % initial capacity even after 9000 cycles.