due to the critical impact on their optoelectronic properties. [2] One example is gels composed of π-conjugated molecules (π-gels). [3] π-Gels are nanocomposites that comprise branched fibers and enclosed solvents. In the fibers, π-conjugated molecules typically assume polycrystalline ordering. Since the charge transport in organic semiconductors is governed by intermolecular interactions, the high crystallinity of π-gels provides preferable electronic properties. π-Gels have been applied to a variety of electronic devices including organic field-effect transistors (OFETs). [4] These supramolecular devices display improved performance in comparison to that of bulk devices. However, integrating supramolecular assemblies into a device still remains elusive, that is, transforming a gel to a device often results in sparsely dispersed fibers. Although individual molecular assemblies display remarkable charge-carrier mobility, the transconductance (g m = ∂I d /∂V g) and the output current by the device unit are far below the practically desired values. Recently, we comprehensively studied the gelation behavior of poly(para-phenyleneethynylene)s (PPEs) and disclosed a

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