We report the synthesis and comprehensive characterization of a dimethylmethylene-bridged N-heterotriangulene (N-HTA) with diaminotriazinyl groups to guide the self-assembly through directional hydrogen bonding. Mass spectrometry collision-induced dissociation experiments indicated the formation of multiply charged clusters in the gas phase. Single crystal X-ray diffraction studies revealed that the solid state packing is governed by an interplay between the hydrogen bonding and the …