Broadband nonlinear optical (NLO) organic nanostructures exhibiting both ultrafast photoresponse and a large cross-section of two-photon absorption throughout a wide NIR spectrum may make them suitable for use as nonlinear biophotonic materials. We report here the synthesis and characterization of two C₆₀-(antenna)(x) analogous compounds as branched triad C₆₀(>DPAF-C₁₈)(>CPAF-C(2M)) and tetrad C₆₀(>DPAF-C₁₈)(>CPAF-C(2M))₂ nanostructures. These compounds showed approximately equal extinction coefficients of optical absorption over 400-550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780-1,100 nm. Accordingly, they may be utilized as potential precursor candidates to the active-core structures of photosensitizing nanodrugs for 2γ-PDT in the biological optical window of 800-1,050 nm.