Differences in molecular structure bestow different chemical properties on the spacer cations. For the synthesis of quasi-2D HPs, this in turn manifests notable differences in chemical interactions with other neighboring chemical species, which profoundly tunes the crystallization behaviors, stability and other functionalities of the matrices. While the control over such behaviors is crucial for designing functional materials, understanding such multi-dimensional properties in the complex materials system merely with classical batch-type investigation workflow falls short of the efficiency and insight needed for advanced material design. Specifically, such manual exploration requires a long and intricate exploration loop, as well as expensive costs. Thus, the progress is deemed to be slow, highly attributed to the difficulty in accurate decision making from limited information at each stage .