The compound of poly(lactic acid) (PLA) and cellulose was made by the emulsion-solvent evaporation technique in order to obtain spheres which are then compression molded to produce a biocomposite film. The effect of the dispersant (poly(vinyl alcohol)—PVA)/PLA ratio on the spheres yield was studied. Moreover, to evaluate the effect of cellulose particle size and surface chemistry on the process yield, unbleached eucalypt kraft pulp and microcrystalline cellulose (MCC), both unmodified and physically or chemically modified were used. PLA/cellulose spheres were characterized regarding its physical properties. It was found that the spheres yield is essentially determined by the PVA/PLA ratio and the percentage of cellulose incorporation is greatly affected by the surface chemistry of cellulose. Regarding the films, DSC runs showed a significant effect of the cellulose type incorporated into PLA matrix on the cold crystallization temperature and on the degree of crystallinity of the biocomposite films. The measurement of tensile properties of the biocomposite films revealed that the strength, elongation at break and toughness (tensile energy absorption at break) of the films incorporating unmodified and chemically modified MCC were substantially improved.