We applied a novel molecular wrapping approach to fullerenyl hybrid triads to minimize solid aggregation in coating thin-film applications. Several C₆₀-(antenna)_x and C₇₀-(antenna)_x analogous compounds having branched hybrid triads C₆₀(>DPAF-C₁₈)(>CPAF-C_2M) and C₇₀(>DPAF-C₂)(>CPAF-C_2M) nanostructures, for example, were applied in the study. The structural design was intended to facilitate the ultrafast fs intramolecular energy-transfer from photoexcited antenna to the C₆₀> cage moiety upon two-photon pumping at either 780 or 980 nm, respectively, for broadband nonlinear optical applications. 2PA characteristics at multiple NIR wavelengths provided support for their suitability in uses that includes the 2PA ability of two antenna, DPAF (700‒850 nm) and CPAF (850‒1100 nm), and the fullerene cage at shorter wavelengths (600‒700 nm). The phenomena can be enhanced by the helical polymer wrapping technique.