In the present work, hybrid super-structured nanomaterials were synthesized by the combination of smectite nanoclays with various carbon-based nanomaterials (graphene oxide, carbon nanotubes and adamantylamine) and were used as nanosupports for the covalent and non-covalent immobilization of laccase from Trametes versicolor (TvL). TvL was successfully immobilized on these hybrid nanomaterials, achieving high immobilization yields (up to 85%), while its conformation remained unaltered upon immobilization. The apparent kinetic constants Vmax and Km of the immobilized enzymes strongly depended on the immobilization procedure and the composition of hybrid nanomaterials. Immobilized TvL preserved up to 50% of its initial activity after 24 h of incubation at 60 °C, while free enzyme was totally deactivated. The TvL-hybrid nanomaterials bioconjugates were efficiently applied for the degradation of various synthetic dyes, exhibiting excellent decolorization capacity, as well as high reusability (up to 11 successive catalytic cycles), providing insights into the use of these bionanoconjugates on applications with environmental, and industrial interest.