The nano-organized LipoParticle assemblies, consisting of polymer particles coated with lipid layers, are investigated with the aim of evidencing the impact of the particle chemical nature on their physicochemical behavior. To this end, these colloidal systems are elaborated from anionic submicrometer poly(styrene) (P(St)) or poly(lactic acid) (PLA) particles, and lipid mixtures composed of zwitterionic 1,2-dipalmitoyl-sn-glycero3-phosphocholine (DPPQ and cationic 1,2-dipalniitoyl-3-trimethylammonium-propane (DPTAP). As revealed by various experimental techniques, such as quasielastic light scattering, potential measurements, transmission electron microscopy, and H-1 NMR spectroscopy, the features of both LipoParticle systems are similar when cationic lipid formulations (DPPC/DPTAP mixtures) are used. This result emphasizes the major role of electrostatic interactions as driving forces in the assembly elaboration process. Conversely, the assemblies prepared only with the zwitterionic DPPC lipid are strongly dependent on the particle chemical nature. The structural characteristics of the assemblies based on PLA particles are not controlled and correspond to aggregates, contrary to P(St) particles. To understand this specific phenomenon, and to consequently improve the final organization of these assemblies which are potentially of great interest in biotechnology and biomedicine, numerous investigations are carried out such as the studies of the impact of the ionic strength and the pH of the preparation media, as well as the presence of ethanol (involved in the PLA particle synthesis) or the mean size of the lipid vesicles. From the resulting data and according to the nature of spherical solid support, hydrophobic effects, hydrogen bonds, or dipole-dipole interactions would also appear to influence the LipoParticle elaboration in the case of zwitterionic lipid formulation.