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A series of robust atomically dispersed solid molecular catalysts based on privileged NHC-metal complexes werereadily fabricated via self-assembly from diverse bis-benzimidazolium salts with selected metal precursors.Among them,the NHC-Ru and NHC-Ir polymers have demonstrated high catalytic activity and excellent stabilityas atomically dispersed solid catalysts in hydrogenation,dehydrogenation,and reductive amination reactionsinvolving a number of biomass platform molecules at very low catalyst loadings.