Spherulitic growth, categorized as central multidirectional growth and unidirectional growth via small-angle branching, has increasingly been explored as a method to improve the flowability and bulk density of needle-like crystals. However, the formation of two categories of spherulites in solutions is still unclear. In this work, the formation mechanism of two categories of spherulite was studied in a supercooled nitroguanidine (NQ) aqueous solution with a small amount of gelatin. It is proposed that spherulitic growth depends on the initial morphology of the crystallite, wherein the gelatin concentration, temperature, and initial supersaturation play a vital role. Gelatin can significantly inhibit NQ nucleation, promote branching, and modify the morphology of NQ subunits. At high initial supersaturation and low temperatures, the aspect ratio of the crystal precursor increases and branching is accelerated, so that the lateral faces provide more branching sites than the end faces to promote the unidirectional growth. In comparison, high temperatures promoting the multipoint branching should be mainly responsible for the formation of cauliflower-like spherulites. Furthermore, the bulk densities of the cauliflower-like and compact spherulites of NQ are about triple those of needle-like crystals and their evolutions were observed. Compared with the reported methods, the macromolecule-induced spherulitic growth of NQ without an organic solvent is a green method and will have a bright future for the design and fabrication of other organic spherulites.