The most significant challenges in LHPs synthesis arise from the fact that LHPs are easily disintegrated in almost any polar solvent due to low lattice formation energy. This limitation precludes various polar chemistries for functionalization and surface coating from being applied to LHPs. Recently, a number of synthetic methods to produce single crystalline LHPs in polar solvents have been reported; however, these methods are limited by slow reaction rate, lack of stoichiometric control, undesirable cracks generated on microcrystals during film detachment, and failure to translate to mass production. This invention generates a new method of crystalline and core-shell LHP synthesis. It utilizes sonochemistry to enable the rapid, large-scale synthesis of various LHPs microstructures in polar aprotic solvents. Such colloidal synthesis enables the full encapsulation of individual LHP microcrystals with polar prepolymers like poly-norepinephrine (pNE). These prepared core-shell structures also show improved optical and structural properties and have functionalizable surfaces.