This paper aims to investigate the effect of different chemical modifications of biocomposites based on poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBH) and aloe vera bio-fibers incorporated at 20 wt%. The fiber surface was modified with alkaline, organosilanes, and combined alkaline/organosilanes. Surface morphology, thermal stability, water absorption capacity, and rheological behavior of the modified biocomposite materials were studied, and the results compared to both unmodified biocomposites and neat PHBH. The study showed that the modified biocomposites with both alkaline and organosilanes exhibited an improved surface morphology, resulting in a good fiber/matrix interfacial adhesion. As a result, increases in complex viscosity, storage modulus, and loss modulus were observed, whereas water absorption was reduced. Thermal stability remained almost unchanged, with the exception of the biocomposite treated with alkaline, where this property decreased significantly. Finally, the coupling of alkaline and organosilane modification is an efficient route to enhance the properties of PHBH biocomposites.