Abstract In this contribution, we report the formation, characterization, and photophysical assessment of hybrid nanostructures realized via a rapid and straightforward covalent functionalization reaction between MoS 2 or WS 2 and a modified C 60 bearing a 1,2‐dithiolane chain. Transmission electron microscopy imaging analysis confirmed that the resulting hybrids are homogeneous at the nanoscale level, effectively suppressing undesired fullerene–fullerene aggregation. X‐ray photoelectron and Raman spectroscopy evidenced the covalent connection between the two species, and thermogravimetry determined the loading of C 60 onto MoS 2 or WS 2 . The MoS 2 – C 60 and WS 2 – C 60 hybrids were stable in liquid media, forming homogeneous inks, which enabled the investigation of thermodynamically feasible, excitonic electron transfer resulting in the formation of MoS 2 •+ –C 60 •‐ and WS 2 •+ –C 60 •‐ radical ion pairs by femtosecond transient absorption spectroscopy. The measured rates were found to be 1.92 × 10 7 s −1 for MoS 2 –C 60 and 3.50 × 10 7 s −1 , respectively, revealing their potential as light energy harvesting materials.