Coupling hydroxides with highly conductive materials has become an effective means to solve their conductivity and stability issues in supercapacitors. Herein, a nanoflower nickel−vanadium layered double hydroxide/graphdiyne (NiV-LDHs/GDY) compound was obtained via a two-step strategy which corrected the shortcomings of poor electrical conductivity and stability of nanoflower NiV-LDHs. The nanoflower NiV-LDHs/GDY occupies a preferable mass-specific capacitance of 1397 F g −1 (1 A g −1 ), rate performance of 70.01% (20 A g −1 ), and durability of 100.00% after 5000 cycles compared to NiV-LDHs. In addition, the NiV-LDHs/GDY//AC ASC reveals a corresponding energy density of 35.42 Wh kg −1 (at a power density of 2602.43 W kg −1 ), and the corresponding energy storage capacity still stays at 80.52% after 6000 cycles. The performance improvement is mainly attributed to the introduction of GDY, which improves the pore structure and charge transfer capacity of NiV-LDHs. Hence, such considerable results suggest that nanoflower NiV-LDHs/GDY could be potential candidate materials for energy storage equipment.