The compositions of hydrogel colloidal crystals are made from mixing an aqueous suspension of poly-N-isopropylacrylamide (“PNIPAM”)-co-allylamine microgels with dichloromethane, forming a PNIPAM-co-allylamine/dichloromethane mixture. The PNIPAM-co-allylamine/dichloromethane mixture is incubated for a period of time at a given temperature, forming the colloidal crystal material. The colloidal crystals can be stabilized by diffusing a glutaric dialdehyde solution into the colloidal crystal material. The concentration of polymer matrix microgels can determine the orientation of random or columnar crystals.