To satisfy the requirements for various highly regarded applications such as electric transportation systems and portable electronic devices, developing advanced energy storage devices with high energy density, power density, and long lifespan is significantly rising. Li-ion batteries (LIBs) and supercapacitors (SCs) are state-of-the-art energy storage technologies owing to their widespread usage in practical applications. However, LIBs and SCs cannot simultaneously meet high energy density, high power density, and long cyclic stability due to their storage mechanism, relying on their active materials. Li-ion hybrid capacitors (LIHCs) have attracted intensive attention due to their high energy and power density and long cyclability. LIHCs are composed of battery-type and capacitor-type electrodes, benefiting from the advantages of both LIBs and SCs. In this chapter, we briefly introduce the principle of LICs, classify battery- and capacitor-type electrode materials, and discuss the criteria for materials selection. Then, recent challenges and developments associated with LIHCs are discussed. Providing in-depth insights into designing electrode materials for LIHCs as the next generation of energy storage devices is the overall aim of this chapter.