Transparent matrices of low refractive index are promising carriers for photoluminescent nanoparticles targeting true volumetric 3D display applications. Complementation of transparency with a highly open-porous nanomorphology renders respective hybrid gels and aerogels additionally attractive for liquid and gas detection devices. Herein, we present virtually fully bio-based hybrids obtained by decorating highly transparent, nematically ordered gels and aerogels (15–20 mg cm−3) from carboxylated and individualized cellulose nanofibers (i-CNF) with amino-functional photoluminescent carbon dots (CD). The latter were obtained by microwave-assisted hydrothermolysis of lemon juice. As the way of anchoring the CDs onto the large internal surface of the porous i-CNF scaffolds (320 m2 g−1) has a great impact on the final properties of the hybrid materials including leaching of CDs and reusability of the hybrid, this study assessed the respective pros and cons of a physical and chemical bonding approach. The results confirmed the superiority of covalent grafting. Aqueous carbodiimide coupling of amino-functionalized CDs afforded higher yields of CDs in the final hybrid aerogels, distinctly higher specific surface values (491 m2 g−1) and slightly enhanced mechanical properties while the high light transmittance and nanomorphology of the i-CNF precursor alcogels is virtually not compromised. Therefore, we conclude that the luminescent i-CNF/CD-chem hybrid materials of this study are promising candidates for environmentally friendly chemical sensing and volumetric display applications.