Supramolecular cross-linking and gelation represent a fascinating approach to improve the performance of pi-conjugated polymers. Up to now, supramolecular pi-conjugated polymer networks have been mainly developed by grafting noncovalent recognition motifs onto the side-chain of pi-conjugated polymers. In comparison, much less attention has been paid to the construction of main-chain-type supramolecular polymer networks, in which pi-conjugated polymers themselves serve as the noncovalent linkages. Herein we have developed a novel and efficient strategy to attain this objective. The design principle is primarily on the basis of noncovalent molecular recognition between bis[alkynylplatinum(II)]terpyridine molecular tweezer receptor and NH-type carbazole guest, which shows enhanced binding affinity due to the cooperative participation of donor-acceptor and intermolecular N-H-N hydrogen-bonding interactions. The "hydrogen-bond enhanced molecular tweezer/guest recognition" strategy can be further applied for multivalent complexation between pi-conjugated polycarbazoles and homoditopic molecular tweezer cross-linker, leading to the formation of main-chain-type supramolecular polymer networks and gels with thermal and solvent responsiveness. Hence, pi-conjugated polymers can be endowed with excellent processability via the supramolecular engineering approach, which provides a new avenue toward flexible optoelectronic applications.