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Concern for the potential global change consequences of increasing atmospheric CO2 has prompted interest in the development of mechanisms to reduce or stabilize atmospheric CO2. During the next several decades, a program focused on terrestrial sequestration processes could make a significant contribution to abating CO2 increases. The reclamation of degraded lands, such as mine-spoil sites, highway rights-of-way, and poorly managed lands, represents an opportunity to couple C sequestration with the use of fossil-fuel and energy by-products and other waste material, such as biosolids and organic wastes from human and animal sewage treatment facilities, to improve soil quality. Degraded lands are often characterized by acidic pH, low levels of key nutrients, poor soil structure, and limited moisture-retention capacity. Much is known about the methods to improve these soils, but the cost of implementation is often a limiting factor. However, the additional financial and environmental benefits of C sequestration may change the economics of land reclamation activities. The addition of energy-related by-products can address the adverse conditions of these degraded lands through a variety of mechanisms, such as enhancing plant growth and capturing of organic C in long-lived soil C pools. This review examines the use of fossil-fuel combustion by-products and organic amendments to enhance C sequestration and identifies the key gaps in information that still must be addressed before these methods can be implemented on an environmentally meaningful scale.