A new methodology to prepare lyophilisomes (self-assembled vesicles composed of phospholipids), which are known as biocapsules, from a range of biomolecules was investigated. The samples used included elastin, acetic acid and liquid nitrogen. The technique involved freezing, annealing, and lyophilization procedure. The transmission electron microscopy (TEM) unveiled the capsule nature of the spheres. The walls of the capsules were found to be smooth with equal distribution of protein over it. Fast-freezing in liquid N2 initiated a micro-phase separation between the bulk of the water and an elastin/acetic acid/water compartment. The transition of the spheres into capsules took place due to coffee-stain mechanism, which explains the formation of solid, ringlike stains from solution droplets. The technique offers enough flexibility and is useful for the development of new biocapsules.