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Li-ion capacitors (LICs) are designed to achieve high power and energy densities using a carbon-based material as a positive electrode coupled with a negative electrode often adopted from Li-ion batteries. However, such adoption cannot be direct and requires additional materials optimization. Furthermore, for the desired device’s performance, a proper design of the electrodes is necessary to balance the different charge storage mechanisms. The negative electrode with an intercalation or alloying active material must provide the high rate performance and long-term cycling ability necessary for LIC functionality—a primary challenge for the design of these energy-storage devices. In addition, the search for new active materials must also consider the need for environmentally friendly chemistry and the sustainable availability of key elements. With these factors in mind, this review evaluates advanced and emerging materials used as high-rate anodes in LICs from the perspective of their practical implementation.