New materials hold the key to fundamental advances in energy conversion and storage, both of which are vital in order to meet the challenge of sustainable and renewable energy sources. Lithium-ion capacitors (LICs) represent an important strategy for electrochemical energy storage, but are usually limited by relatively low energy density. In this study we assembled a hybrid LIC featuring a bulk graphdiyne (GDY) anode and an activated carbon (AC) cathode. This capacitor delivered an initial specific energy as high as 112.2Whkg–1 at a power density of 400.1Whkg–1, with 94.7% retention after 1000 cycles. More importantly, it even displayed an energy density of 95.1Whkg−1 at a power density of 1000.4Wkg–1, operated in the voltage range of 2–4V. Those high energy and power densities in LICs constructed with GDY anode and AC cathode offer a great potential toward application on next generation batteries.