In fact, the chemical variability of spacer cations offers an infinite molecular space, making the systematic and comprehensive investigation of the supramolecular interaction difficult. Particularly, due to the coexistence and interplays of multiple physicochemical parameters of molecular spacer affecting HP crystallizations, manual exploration to resolve such a multi-faceted problem is extremely challenging. Moreover, the chemistry in the vast molecular spaces is -inherently -discrete, rather than continuous landscapes. Thus, for optimizing the optoelectronic functionalities of the quasi-2D HPs, seamless navigation of such intricate chemical space is necessary, which is also difficult based on the classical, single-directional process refinement techniques.