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High dielectric constants in organic semiconductors have been identified as a central challenge for the improvement in not only piezoelectric, pyroelectric, and ferroelectric effects but also photoelectric conversion efficiency in OPVs, carrier mobility in OFETs, and charge density in charge-trapping memories. Herein, we report an ultralong persistence length (    l    p    ≈  41   nm) effect of spiro-fused organic nanopolymers on dielectric properties, together with excitonic and charge carrier behaviors. The state-of-the-art nanopolymers, namely, nanopolyspirogrids (NPSGs), are synthesized via the simple cross-scale Friedel-Crafts polygridization of A 2 B 2 -type nanomonomers. The high dielectric constant (  k  =  8.43  ) of NPSG is firstly achieved by locking spiro-polygridization effect that results in the enhancement of dipole polarization. When doping into a polystyrene-based dielectric layer, such a high-  k   feature of NPSG increases the field-effect carrier mobility from 0.20 to 0.90 cm 2  V -1  s -1  in pentacene OFET devices. Meanwhile, amorphous NPSG film exhibits an ultralow energy disorder (&lt;50 meV) for an excellent zero-field hole mobility of   3.94  ×    10    −  3       c    m    2         V    −  1         s    −  1    , surpassing most of the amorphous   π  -conjugated polymers. Organic nanopolymers with high dielectric constants open a new way to break through the bottleneck of efficiency and multifunctionality in the blueprint of the fourth-generation semiconductors.

Cross-Scale Synthesis of Organic High-k Semiconductors Based on Spiro-Gridized Nanopolymers