In the paper, residual-layer-free nanoimprint lithography for large-area fabrication is reviewed. In order to remove the residual layer during the imprint process, polymer resists and mold materials should be designed with the aspects of surface chemistry and mold geometries in mind. Various approaches for residual-layer-free nanoimprint lithography are discussed including incomplete filling by polymer mass, reverse imprint methods, self-removal techniques, and the employment of elastomeric mold deformation. In addition, issues that must be overcome to enable large-area roll-to-roll nanoimprinting without a residual layer are presented.