Organic grido-architectures offer not only state-of-the-art models for exploring the complex relationships of multicarrier coherence among excitons, charges, photons, electrons, and phonons but also organic high-dimensional nanomaterials for flexible electronics and organic intelligence. Herein, we initiate the fundamental progress and perspective on gridofluorene-based zero-, one-, two-, and three-dimensional nanomolecules and their optoelectronic features. From the future point of view, the sterically trans-dimensional and hierarchically cross-scale effects of these covalent frameworks and nanostructures are discussed on their photophysical, electrical, mechanical and thermal properties. Organic multiscale systems, with the feature of synergistically molecule-programmable integration of diverse functionalities, open a bright door to flexible electronics, intelligent molecules, devices, systems, and even organobots as well as artificially intelligent and robotic chemists (AiRCs).