Near-infrared (NIR) organic materials are of great importance for both fundamental research and practical applications. While much effort has been taken to covalently design and synthesize NIR organic materials with a low energy gap, there are supramolecular approaches for tuning the energy gap to noncovalently fabricate NIR organic assemblies and materials. In this concept article, we summarize and discuss several supramolecular approaches, including the fabrication of charge transfer supramolecular complexes, the fabrication of supramolecular J-aggregates, and the fabrication of supramolecularly stabilized organic radicals. The nature of noncovalent interactions in supramolecular approaches can provide NIR organic assemblies and materials with unique properties such as reversibility, stimuli-responsiveness, recyclability, and adaptive abilities.